Co-reporter:Lile Dong, Peng Zhang, Pengpeng Lei, Shuyan Song, Xia Xu, Kaimin Du, Jing Feng, and Hongjie Zhang
ACS Applied Materials & Interfaces June 21, 2017 Volume 9(Issue 24) pp:20426-20426
Publication Date(Web):May 30, 2017
DOI:10.1021/acsami.7b04438
Contrast agents for multimodal imaging are in high demand for cancer diagnosis. To date, integration of T1/T2-weighted magnetic resonance imaging (MRI) and X-ray computed tomography (CT) imaging capabilities in one system to obtain an accurate diagnosis still remains challenging. In this work, biocompatible PEGylated GdF3:Fe nanoparticles (PEG-GdF3:Fe NPs) were reasonable designed and synthesized as multifunctional contrast agents for efficient T1/T2-weighted MRI and X-ray CT multimodal imaging. Owing to the enhanced permeability and retention effect in vivo, strong T1 contrast, evident T2 contrast, and X-ray CT signals in a tumor lesion can be observed after intravenous injection of PEG-GdF3:Fe NPs. Therefore, PEG-GdF3:Fe NPs could be used as potential multimodal contrast agents for cancer diagnosis.Keywords: multimodal; PEG-GdF3:Fe NPs; T1/T2-weighted MRI; X-ray CT imaging;
Co-reporter:Rongzhen Cui, Weiqiang Liu, Liang Zhou, Yanan Li, Yunlong Jiang, Xuesen Zhao, Yingjie Cui, Qi Zhu, Youxuan Zheng, Ruiping Deng, Hongjie Zhang
Dyes and Pigments 2017 Volume 136() pp:361-367
Publication Date(Web):January 2017
DOI:10.1016/j.dyepig.2016.08.068
•Tb(acac)3(phen-Cl) was utilized as sensitizer for the first time in phosphorescent OLEDs.•Tb(acac)3(phen-Cl) exhibited low-lying energy levels and high triplet energy of ligand.•No Tb(III) ion emission was observed in co-doped devices.•Tb(acac)3(phen-Cl) co-doped devices obtained higher brightness, higher efficiencies and even slower efficiency roll-off.An effective device design strategy was reported to realize high performance green organic light-emitting diodes based on iridium complex by employing a trivalent terbium complex as the sensitizer. The low-lying energy levels of utilized terbium complex are beneficial in broadening recombination zone and facilitating carriers' balance on emitter molecules. No terbium ion characteristic emission was observed in co-doped devices ascribed to high triplet energy of the ligand of terbium complex. Consequently, the 0.4 wt% co-doped single light-emitting layer device obtained the maximum external quantum efficiency, current efficiency and power efficiency up to 27.6%, 114.23 cd/A and 101.92 lm/W, respectively. At 3.8 V, this device realized the practical brightness of 1000 cd/m2 with inspiring external quantum efficiency and current efficiency as high as 27.5% and 113.71 cd/A, respectively. While the 0.2 wt% co-doped double light-emitting layers device displayed relatively lower efficiency, but higher brightness up to 205,629 cd/m2.
Co-reporter:Rongzhen Cui;Weiqiang Liu;Liang Zhou;Xuesen Zhao;Yunlong Jiang;Youxuan Zheng;Hongjie Zhang
Journal of Materials Chemistry C 2017 vol. 5(Issue 8) pp:2066-2073
Publication Date(Web):2017/02/23
DOI:10.1039/C6TC05542G
In this work, we demonstrated the efficacy and feasibility of utilizing terbium and gadolinium complexes with low-lying energy levels to sensitize red-emitting iridium complexes in organic light-emitting diodes (OLEDs). Compared with devices without the introduction of a sensitizer, the obtained sensitized devices showed remarkably enhanced electroluminescence performances, which can be attributed to improved carrier balance as well as a wider recombination zone. Moreover, characteristic sensitizer emission was invisible in all sensitized devices due to the inferior hole trapping ability of sensitizer molecules. Finally, the sensitized device co-doped with 0.4 wt% of the terbium complex realized superior electroluminescence performances with maximum brightness, current efficiency, power efficiency and external quantum efficiency as high as 145 071 cd m−2, 64.87 cd A−1, 69.11 lm W−1 and 24.7%, respectively. Meanwhile, even at the practical brightness of 1000 cd m−2 (4.0 V), outstanding external quantum efficiency and current efficiency up to 22.7% and 59.7 cd A−1, respectively, were obtained.
Co-reporter:Xia Xu;Yan Long;Pengpeng Lei;Lile Dong;Kaimin Du;Jing Feng;Hongjie Zhang
Journal of Materials Chemistry C 2017 vol. 5(Issue 37) pp:9666-9672
Publication Date(Web):2017/09/28
DOI:10.1039/C7TC02665J
We report a hybrid assembly based on NaYF4:Yb3+,Er3+/Tm3+@NaYF4 (core@shell) upconversion nanocrystals and ultrasmall Ni nanoparticles (abbreviated as core@shell@Ni) for rapid response towards pH in different PBS solutions. In this approach, Ni nanoparticles located on the surface of the core@shell upconversion nanocrystal serve as an efficient quencher for upconversion luminescence (UCL). A series of dynamic processes of the 4S3/2 → 4I15/2 transition of Er3+ in Er3+-doped core@shell@Ni have been presented in order to discuss the energy transfer mechanisms between UCNPs and Ni nanoparticles. The upconversion luminescence can be recovered by incubating the core@shell@Ni assembly with pH 5.0 PBS that oxidizes Ni to Ni2+, while the UCL could be still quenched when the hybrid assembly was incubated with pH 7.4 PBS. However, the core@shell@Co assembly's response toward pH is not distinguished due to the rapid recovery of emission intensity both in pH 5.0 and 7.4 PBS. The ability of the core@shell@Ni assembly to distinguish different pH values may be a fine platform for the real-time optical monitoring of chemical reactions and many important physiological processes associated with pH.
Co-reporter:Pengpeng Lei;Ran An;Shuang Yao;Qishun Wang;Lile Dong;Xia Xu;Kaimin Du;Jing Feng;Hongjie Zhang
Advanced Materials 2017 Volume 29(Issue 22) pp:
Publication Date(Web):2017/06/01
DOI:10.1002/adma.201700505
Upconversion (UC) nanoparticles (UCNPs) have evoked considerable attention in many fields owing to their fascinating features. However, rigorous synthesis conditions and expensive raw materials often limit their further applications. Here, a novel hexagonal phase NaBiF4 UC matrix through a very facile method (one min only at room temperature) is synthesized. The nanoparticles show good monodispersity with uniform size. Under the 980 nm irradiation, Yb3+/Ln3+ (Ln = Er, Ho, Tm) codoped NaBiF4 nanoparticles show excellent UC luminescence (UCL). This super facile synthesis strategy and excellent matrix materials enable to achieve UCL in such low temperature, opening a new gateway for the UCNPs applied to a variety of areas in the future.
Co-reporter:Shuyan Song;Xianchun Liu;Junqi Li;Jing Pan;Fan Wang;Yan Xing;Xiao Wang;Xiaogang Liu;Hongjie Zhang
Advanced Materials 2017 Volume 29(Issue 28) pp:
Publication Date(Web):2017/07/01
DOI:10.1002/adma.201700495
Ultrathin (Pt-enriched cage)@CeO2 core@shell nanostructures are successfully fabricated via a facile hard-template method. It is found that the usage of Pd@Ag@CeO2 bi-metallic core@shell nanostructure as the hard template plays an important role in avoiding the independent nucleation of Pt metal during the galvanic replacement process between K2PtCl4 and Ag components. This unique core@shell samples show extraordinary activity and selectivity for the cinnamaldehyde hydrogenation reaction. It can achieve over 95% conversion with 87% selectivity of hydrocinnamaldehyde in 5 h under 1 atm H2 pressure. It is considered that such high catalytic performance could be attributed to the densely CeO2-coated core@shell hybrid form as well as the ultrathin nature of the Pt-enriched cage.
Co-reporter:Pengpeng Lei;Ran An;Peng Zhang;Shuang Yao;Shuyan Song;Lile Dong;Xia Xu;Kaimin Du;Jing Feng;Hongjie Zhang
Advanced Functional Materials 2017 Volume 27(Issue 35) pp:
Publication Date(Web):2017/09/01
DOI:10.1002/adfm.201702018
To elaborately fabricate real-time monitoring and therapeutic function into a biocompatible nanoplatform is a promising route in the cancer therapy field. However, the package of diagnosis and treatment into a single-“element” nanoparticle remains challenge. Herein, ultrasmall poly(vinylpyrrolidone)-protected bismuth nanodots (PVP-Bi nanodots) are successfully synthesized through an ultrafacile strategy (1 min only under ambient conditions). The nanodots are easy to synthesize in both laboratory and large scale using low-cost bismuth ingredients. PVP-Bi nanodots with ultrasmall size show good biocompatibility. Due to the high X-ray attenuation ability of Bi element, PVP-Bi nanodots have prominent performance on X-ray computed tomography (CT) imaging. Moreover, PVP-Bi nanodots exhibit a high photothermal conversion efficiency (η = 30%) because of the strong near-infrared absorbance, which can serve as nanotheranostic agent for photothermal imaging and cancer therapy. The subsequent PVP-Bi-nanodot-mediated photothermal therapy (PTT) result shows highly efficient ablation of cancer cells both in vitro and in vivo. PVP-Bi nanodots can be almost completely excreted from mice after 7 d. Blood biochemistry and histology analysis suggests that PVP-Bi nanodots have negligible toxicity. All the positive results reveal that PVP-Bi nanodots produced through the ultrafacile method are promising single-“element” nanotheranostic platform for dual-modal CT/photothermal-imaging-guided PTT.
Co-reporter:Fan Wang;Shuyan Song;Junqi Li;Jing Pan;Xiao Wang;Hongjie Zhang
Nanoscale (2009-Present) 2017 vol. 9(Issue 19) pp:6346-6352
Publication Date(Web):2017/05/18
DOI:10.1039/C7NR01665D
A facile route for the synthesis of a type of composite nanotube, namely S,N co-doped carbon nanotubes decorated with molybdenum disulfide nanosheets (CP/MoS2), is now reported. The number of nanosheets for MoS2 can be easily tuned by changing the templates with different ratios of N and S. When evaluated as an anode material for lithium-ion batteries, the CP/MoS2 nanotubes show a high specific capacity of around 1500 mA h g−1 at the current density of 50 mA g−1, excellent cycling stability up to 750 cycles at the current density of 1 A g−1, and superior rate performance.
Co-reporter:Fan Wang;Shuyan Song;Junqi Li;Jing Pan;Xiao Wang;Hongjie Zhang
Nanoscale (2009-Present) 2017 vol. 9(Issue 19) pp:6346-6352
Publication Date(Web):2017/05/18
DOI:10.1039/C7NR01665D
A facile route for the synthesis of a type of composite nanotube, namely S,N co-doped carbon nanotubes decorated with molybdenum disulfide nanosheets (CP/MoS2), is now reported. The number of nanosheets for MoS2 can be easily tuned by changing the templates with different ratios of N and S. When evaluated as an anode material for lithium-ion batteries, the CP/MoS2 nanotubes show a high specific capacity of around 1500 mA h g−1 at the current density of 50 mA g−1, excellent cycling stability up to 750 cycles at the current density of 1 A g−1, and superior rate performance.
Co-reporter:Yanan Li;Liang Zhou;Yunlong Jiang;Rongzhen Cui;Xuesen Zhao;Hongjie Zhang
Journal of Materials Chemistry C 2017 vol. 5(Issue 17) pp:4219-4225
Publication Date(Web):2017/05/04
DOI:10.1039/C7TC00725F
In this work, we demonstrated a novel device design strategy to obtain efficient pure blue organic fluorescent electroluminescent (EL) devices by doping a traditional electron transport material, 9,10-bis[4-(6-methylbenzothiazol-2-yl)phenyl]anthracene (DBzA), into a hole transporting host material, 4,4′,4′′-tris(carbazol-9-yl)-triphenylamine (TcTa), as the light-emitting layer (EML). Here, DBzA functions not only as a blue emitter but also as an electron transport material. Due to the well matched energy levels of DBzA and TcTa, the obtained devices displayed a broadened recombination zone, improved trapping of carriers, and balanced distribution of holes and electrons on emitter molecules. Interestingly, a single-EML device displayed higher EL efficiencies and lower operation voltage than those of a double-EML device. Finally, a pure blue EL device (Commission Internationale de l'Eclairage (CIE) coordinates of (0.141, 0.165)) with maximum brightness, current efficiency, power efficiency and external quantum efficiency (EQE) of up to 10 384 cd m−2, 6.41 cd A−1, 6.71 lm W−1, and 4.3%, respectively, was realized by optimizing the doping concentration. Even at a certain brightness of 1000 cd m−2, current efficiency as high as 4.1 cd A−1 (EQE = 2.8%) can be retained by the same device.
Co-reporter:Xia Xu;Xuesong Zhai;Kaimin Du;Pengpeng Lei;Lile Dong;Ruiping Deng;Jing Feng;Hongjie Zhang
Journal of Materials Chemistry C 2017 vol. 5(Issue 25) pp:6311-6318
Publication Date(Web):2017/06/29
DOI:10.1039/C7TC01586K
Impurity doping has a significant influence on the nucleation and growth of nanocrystals. The influence of the ionic radius of the dopant and grain size on the crystallographic phase of KLu2F7:Yb3+/Er3+ nanocrystals has not been systematically investigated. Herein, we demonstrate an M ion (M = Mn2+, Gd3+, Nd3+) doping approach to dynamically fine-tune the grain size of KLu2F7:Yb3+/Er3+ nanocrystals, and study the influence of the ionic radius of the doping M ions and particle size reduction on the crystallographic phase. Through a comprehensive investigation of the impurity doping induced phase transition phenomenon and the growth mechanism of KLu2F7:Yb3+/Er3+ nanocrystals, we speculated that the impurity doping induced phase transition mechanism of KLu2F7:Yb3+/Er3+ mainly depends on the grain size of nanocrystals ignoring the ionic radius of the dopant. With the decrease of the grain size, high surface tension triggers phase transformation from anisotropic (orthorhombic KLu2F7:Yb3+/Er3+) to isotropic (cubic KLu3F10:Yb3+/Er3+). What is more, we have systematically investigated the visible (VIS)-upconversion and near infrared (NIR)-downshifting emission of various-sized KLu2F7:Yb3+/Er3+ UCNPs and Mn2+, Gd3+ or Nd3+ ion doped KLu2F7:Yb3+/Er3+ UCNPs. The findings provide keen insights into understanding the effect of size reduction on the phase transition mechanism and the photoluminescence properties of KLu2F7:Yb3+/Er3+ UCNPs, while offering the possibility for good academic studies and application prospects.
Co-reporter:Pengpeng Lei;Ran An;Xuesong Zhai;Shuang Yao;Lile Dong;Xia Xu;Kaimin Du;Manli Zhang;Jing Feng;Hongjie Zhang
Journal of Materials Chemistry C 2017 vol. 5(Issue 37) pp:9659-9665
Publication Date(Web):2017/09/28
DOI:10.1039/C7TC03122J
Upconversion luminescent materials have received much attention due to their unique luminescence properties and potential applications in various fields. However, the weak upconversion luminescence (UCL) intensity and low quantum yield often limit their development. Herein, Yb3+/Er3+(Tm3+) codoped NaBiF4 upconversion nanoparticles (UCNPs) have been successfully synthesized through a facile one-pot solvothermal method. Under 980 nm excitation, NaBiF4:Yb3+/Er3+(Tm3+) UCNPs show excellent UCL. The UCL intensities of NaBiF4:Yb3+/Er3+ and NaBiF4:Yb3+/Tm3 UCNPs could be further enhanced through polyacrylic acid (PAA) modification on the surface to be 4.2 and 3.1 times stronger than those of their unmodified counterparts, respectively. The UCL quantum yields of the PAA-modified NaBiF4 UCNPs are 0.32% (Er3+) and 3.70% (Tm3+), which are higher than those of the unmodified NaBiF4:Yb3+/Er3+(Tm3+) UCNPs and NaYF4:Yb3+/Er3+(Tm3+) UCNPs (the most efficient UC materials). Moreover, the temperature-dependent UCL properties of NaBiF4:Yb3+/Er3+ and PAA-modified NaBiF4:Yb3+/Er3+ were investigated systematically under 980 nm excitation. The modification of PAA on the surface of the NaBiF4:Yb3+/Er3+ UCNPs could effectively improve the fit degree (r2 value) of the experimental data and the maximum thermal sensitivity of PAA-modified NaBiF4:Yb3+/Er3+ could reach 0.0040 K−1 at 498 K. Therefore, PAA-modified NaBiF4:Yb3+/Er3+ UCNPs with strong UCL and high quantum yield could be a potential candidate for sensitive temperature sensors.
Co-reporter:Xing Meng;Hai-Ning Wang;Shu-Yan Song;Hong-Jie Zhang
Chemical Society Reviews 2017 vol. 46(Issue 2) pp:464-480
Publication Date(Web):2017/01/23
DOI:10.1039/C6CS00528D
Crystalline porous materials are currently a hot research topic in the field of proton-conducting materials. Crystalline porous materials include metal–organic frameworks (MOFs), coordination polymers (CPs), polyoxometalates (POMs) and covalent organic frameworks (COFs). The designable structures and high surface areas of these materials provide great opportunities to orderly accommodate proton carriers and to systemically modify the concentration and mobility of proton carriers in available spaces. Based on the understanding of the relationship between the structure and proton conductivity, controllable synthesis of porous materials with high proton conductivity will gradually be achieved. This review summarizes the emerging studies of these materials and their unique proton conductivities.
Co-reporter:Junqi Li;Xiao Wang;Shuyan Song;Shu'na Zhao;Fan Wang;Jing Pan;Jing Feng;Hongjie Zhang
CrystEngComm (1999-Present) 2017 vol. 19(Issue 11) pp:1459-1463
Publication Date(Web):2017/03/13
DOI:10.1039/C6CE02616H
Unique self-supported arrays (Co3O4 nanowire-self-penetrated-Co3O4 nanocages) on Ni foam are successfully fabricated via a metal–organic-framework (MOF)-assisted method. The as-obtained sample exhibits a remarkably enhanced supercapacitance performance.
Co-reporter:Junqi Li;Xiao Wang;Shuyan Song;Shu'na Zhao;Fan Wang;Jing Pan;Jing Feng;Hongjie Zhang
CrystEngComm (1999-Present) 2017 vol. 19(Issue 11) pp:1459-1463
Publication Date(Web):2017/03/13
DOI:10.1039/C6CE02616H
Unique self-supported arrays (Co3O4 nanowire-self-penetrated-Co3O4 nanocages) on Ni foam are successfully fabricated via a metal–organic-framework (MOF)-assisted method. The as-obtained sample exhibits a remarkably enhanced supercapacitance performance.
Co-reporter:Yingbo Liu;Liang Zhou;Yanan Li;Ruiping Deng;Hongjie Zhang
Nanoscale (2009-Present) 2017 vol. 9(Issue 2) pp:491-496
Publication Date(Web):2017/01/05
DOI:10.1039/C6NR07123F
High quantum yields (QY) and stable performances are prerequisites for implementing carbon dots in practical applications. In this study, we demonstrate that nitrogen-doped carbon dots (N-CDs), which were prepared via the hydrothermal treatment of citric acid (CA) and tris(hydroxymethyl)methyl aminomethane (Tris), have a high QY of 75%, together with excellent thermal and photo stability. These N-CDs deliver an excellent thermal stability performance over the temperature range of 25 °C to 95 °C, and even at a heating temperature of 90 °C for 360 min. Upon exposure to UV illumination with a radiant intensity of 20 mW cm−2, 96% fluorescence intensity is retained. This florescence stability performance is probably due to the chemical composition and steric effect of the nitrogen-doping agent. Furthermore, the remarkable optical properties of these N-CDs allow them to be used as invisible ink for loading important information and advanced anti-counterfeiting.
Co-reporter:Yinghui Wang, Xing Ding, Fan Wang, Junqi Li, Shuyan Song and Hongjie Zhang
Chemical Science 2016 vol. 7(Issue 7) pp:4284-4290
Publication Date(Web):09 Mar 2016
DOI:10.1039/C5SC04668H
To tackle the issues of inferior cycling stability and low conductivity for MnO as an anode material for lithium ion batteries (LIBs) and as a catalyst for oxygen reduction reaction (ORR), a facile and effective strategy is explored to confine N-doped carbon-coated MnO nanoparticles in a conductive graphene matrix. The synthesis of the GMNCs involves the two-step coating of Mn3O4 nanocrystals with polydopamine and graphene, followed by heat treatment to form the GNS@MnO@N-doped carbon composites (GMNCs). When evaluated as anode materials for LIBs, the as-prepared GMNCs exhibit an improved cycling stability (754.3 mA h g−1 after 350 cycles at 0.1 A g−1) compared to carbon-coated MnO and pure Mn3O4 due to the double carbon coating design. When evaluated as catalysts for ORR, the as-prepared GMNCs exhibit higher electrocatalytic activity than that of pure Mn3O4 and MnO catalysts, and superior stability to a commercial Pt/C catalyst due to the synergetic effect between the MnO and N-doped double carbon coating. The optimum design of the unique nanostructures with the synergetic effect provides a new route to design advanced materials as electrode/catalysts for energy conversion and storage.
Co-reporter:Xiao Wang, Shuna Zhao, Yibo Zhang, Zhuo Wang, Jing Feng, Shuyan Song and Hongjie Zhang
Chemical Science 2016 vol. 7(Issue 2) pp:1109-1114
Publication Date(Web):28 Oct 2015
DOI:10.1039/C5SC03430B
Recently, mixed metal oxides have attracted tremendous interest because of their great importance for fundamental studies and practical applications in the catalytic field to replace expensive noble metals. Herein, we report the designed synthesis of novel CeO2–Co3O4 mixed metal oxides with complex nanostructures using uniform short CeO2 nanowires self-inserted into ZIF-67 nanocrystals as precursors followed by a thermal annealing treatment. Interestingly, such a synthetic strategy can be easily extended to fabricate other CeO2 nanowires inserted into metal oxide nanoframeworks such as NiCo2O4 and ZnCo2O4. Choosing the NO reduction reaction by CO as the catalytic model, the as-obtained CeO2–Co3O4 hybrids exhibited enhanced catalytic performance, which could be attributed to the strong two-phase interaction between each component.
Co-reporter:Pengpeng Lei, Peng Zhang, Shuang Yao, Shuyan Song, Lile Dong, Xia Xu, Xiuling Liu, Kaimin Du, Jing Feng, and Hongjie Zhang
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 41) pp:27490
Publication Date(Web):October 3, 2016
DOI:10.1021/acsami.6b08335
Bioimaging probes have been extensive studied for many years, while it is still a challenge to further improve the image quality for precise diagnosis in clinical medicine. Here, monodisperse NaGdF4:Yb3+,Tm3+,x% Bi3+ (abbreviated as GYT-x% Bi3+, x = 0, 5, 10, 15, 20, 25, 30) upconversion nanoparticles (UCNPs) have been prepared through the solvothermal method. The near-infrared upconversion emission intensity of GYT-25% Bi3+ has been enhanced remarkably than that of NaGdF4:Yb3+,Tm3+ (GYT) with a factor of ∼60. Especially, the near-infrared upconversion emission band centered at 802 nm is 150 times stronger than the blue emission band of GYT-25% Bi3+ UCNPs. Such high ratio of NIR/blue UCL intensity could reduce the damage to tissues in the bioimaging process. The possibility of using GYT-25% Bi3+ UCNPs with strong near-infrared upconversion emission for optical imaging in vitro and in vivo was performed. Encouragingly, the UCL imaging penetration depth can be achieved as deep as 20 mm. Importantly, GYT-25% Bi3+ UCNPs exhibit a much higher X-ray computed tomography (CT) contrast efficiency than GYT and iodine-based contrast agent under the same clinical conditions, due to the high X-ray attenuation coefficient of bismuth. Hence, simultaneous remarkable enhancement of NIR emission and X-ray CT signal in upconversion nanoparticles could be achieved by optimizing the doping concentration of Bi3+ ions. Additionally, Gd3+ ions in the UCNPs endow GYT-25% Bi3+ UCNPs with T1-weighted magnetic resonance (MR) imaging capability.Keywords: Bi3+ ion; NaGdF4; signal enhancement; trimodal imaging; upconversion nanoparticles
Co-reporter:L.B. Tong, J.B. Zhang, C. Xu, X. Wang, S.Y. Song, Z.H. Jiang, S. Kamado, L.R. Cheng, H.J. Zhang
Carbon 2016 Volume 109() pp:340-351
Publication Date(Web):November 2016
DOI:10.1016/j.carbon.2016.08.032
The poor corrosion and wear resistances hinder the industrial applications of magnesium and its alloys. In this paper, a new graphene oxide (GO) coating is fabricated on the surface of extruded Mg-Zn-Ca alloy, via the silane coupling agent. The GO coating has fully covered the Mg substrate through the chemical reactions, and formed an overlapped multilayer structure by interlocked effects. Electrochemical measurements indicate that the anti-corrosion performance can be remarkably improved by silane/GO coating, because the stable covalent bonds within the coating effectively restrict the penetration of electrolyte into the Mg surface, representing an excellent corrosion barrier effect. The GO coating drastically promotes the wear resistance, due to the superior bonding between the Mg substrate and GO sheets with high hardness and good lubricant effect.
Co-reporter:Yunlong Jiang, Liang Zhou, Rongzhen Cui, Yanan Li, Xuesen Zhao, Hongjie Zhang
Dyes and Pigments 2016 Volume 128() pp:26-32
Publication Date(Web):May 2016
DOI:10.1016/j.dyepig.2016.01.011
•Pure red electroluminescent devices with stepwise energy levels were designed and fabricated.•Wide energy gap iridium complex with matched triplet energy was chosen as sensitizer.•The incorporation of sensitizer facilitates the balance of carriers on emitter molecules.•The incorporation of sensitizer broadens the recombination zone.In this work, we report the realization of highly efficient pure red organic co-doped electroluminescent device with tris(1-phenyl-isoquinoline) iridium(III) (Ir(piq)3) and iridium(III) bis(4,6-(difluorophenyl)pyridinato-N,C2′)picolinate (FIrpic) as emitter and sensitizer, respectively. By selecting 4,4′,4″-Tri(9-carbazoyl)triphenylamine and 2,6-bis(3-(9H-carbazol-9-yl)phenyl)pyridine as host materials, a series of devices with single or double light-emitting layer(s) were fabricated and investigated. The well-known wide gap blue emitter FIrpic, which possesses low-lying energy levels, was co-doped minutely into electron dominant light-emitting layer. Compared with reference devices, co-doped devices displayed significant improvement of device performances attributed to improved carriers' balance and broadening recombination zone. Finally, the 0.3 wt% co-doped double light-emitting layers device obtained the maximum brightness, current efficiency, power efficiency and external quantum efficiency up to 28,031 cd/m2, 14.89 cd/A, 12.99 lm/W and 9.0%, respectively. Even at the certain brightness of 1000 cd/m2, EL efficiency as high as 12.06 cd/A can be retained by the same device.Pure red electroluminescent devices with stepwise energy levels were designed and fabricated by co-doping the wide energy gap iridium complex as sensitizer. Significantly improved device performances were realized attributed to improved carriers' balance and broadening recombination zone.
Co-reporter:Junqi Li, Shuang Yao, Shuyan Song, Xiao Wang, Yinghui Wang, Xing Ding, Fan Wang and Hongjie Zhang
Dalton Transactions 2016 vol. 45(Issue 28) pp:11522-11527
Publication Date(Web):20 Jun 2016
DOI:10.1039/C6DT02044E
Nanomaterials that can restrain or reduce the production of excessive reactive oxygen species such as H2O2 to defend and treat against Alzheimer's disease (AD) have attracted much attention. In this paper, we adopt the strategy of layer-by-layer deposition; namely, first synthesizing available gadolinium-doped ytterbia nanoparticles (Yb2O3:Gd NPs) as cores, and then coating them with silica via the classical Stöber method to prevent leakage and act as a carrier for subsequent ceria deposition and PEGylation, and finally obtain the expected core@shell-structured nanocomposite of PEGylated Yb2O3:Gd@SiO2@CeO2 islands. The nanomaterial has proved not only to be a high-performance dual-modal contrast agent for use in MRI and CT, but also to exhibit excellent catalase mimetic activity, which may help the prognosis, diagnosis and treatment of AD in the future. In addition, scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared (FTIR) spectroscopy characterization have revealed the successful design and synthesis of the cores with remarkable size uniformity, with well-distributed CeO2 islands decorated on the surface of SiO2 shells, and tightly immobilized PEG.
Co-reporter:Yue Su, Xiuling Liu, Pengpeng Lei, Xia Xu, Lile Dong, Xianmin Guo, Xingxu Yan, Peng Wang, Shuyan Song, Jing Feng and Hongjie Zhang
Dalton Transactions 2016 vol. 45(Issue 27) pp:11129-11136
Publication Date(Web):21 Jun 2016
DOI:10.1039/C6DT01005A
Core–shell–shell heterostructures of α-NaLuF4:Yb/Er@NaLuF4:Yb@MF2 (M = Ca, Sr, Ba) have been successfully fabricated via the thermal decomposition method. Upconversion nanoparticles (UCNPs) were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), upconversion luminescence (UCL) spectroscopy, etc. Under 980 nm excitation, the emission intensities of the UCNPs are remarkably enhanced after coating the MF2 (M = Ca, Sr, and Ba) shell. Among these samples, CaF2 coated UCNPs show the strongest overall emission, while BaF2 coated UCNPs exhibit the longest lifetime. These results demonstrate that alkaline earth metal fluorides are ideal materials to improve the UCL properties. Meanwhile, although the lattice mismatch between the ternary NaREF4 core and the binary MF2 (M = Sr and Ba) shell is relatively large, the successfully synthesized NaLuF4:Yb/Er@NaLuF4:Yb@MF2 indicates a new outlook on the fabrication of heterostructural core–shell UCNPs.
Co-reporter:Xia Xu, Pengpeng Lei, Lile Dong, Xiuling Liu, Yue Su, Shuyan Song, Jing Feng and Hongjie Zhang
Dalton Transactions 2016 vol. 45(Issue 20) pp:8440-8446
Publication Date(Web):15 Apr 2016
DOI:10.1039/C6DT00707D
Controlling excitation and emission wavelengths on demand is very significant in bioimaging. Up-conversion nanoparticles (UCNPs) emit visible light upon near-infrared (NIR) light excitation and are well studied in bioimaging. Red emission is usually preferred to green due to its higher tissue penetration depth in bioimaging. Herein, dominant red emission has been achieved under 808 nm excitation based on the designed α-NaYbF4:Mn2+/Er3+@NaLuF4:Mn2+/Yb3+@NaNdF4:Yb3+@NaGdF4 (C@S1@S2@S3) nanostructure. The rationally designed interlayer shell NaLuF4:Mn2+/Yb3+ could efficiently filter unwanted energy back-transfer from Er3+ to Nd3+ and the outmost shell NaGdF4 could prevent excitation energy from surface-related quenching. The lifetime of 4F9/2 → 4I15/2 transition of Er3+ could be as high as 0.7 ms. Moreover, C@S1@S2@S3 UCNPs also possess effective contrast efficiency for both X-ray computed tomography (CT) and magnetic resonance (MR) imaging. The designed multifunctional UCNPs could be used as a potential multimodal bioprobe in bioimaging applications.
Co-reporter:Pengpeng Lei, Xiuling Liu, Lile Dong, Zhuo Wang, Shuyan Song, Xia Xu, Yue Su, Jing Feng and Hongjie Zhang
Dalton Transactions 2016 vol. 45(Issue 6) pp:2686-2693
Publication Date(Web):23 Dec 2015
DOI:10.1039/C5DT04279H
Water-soluble lanthanide (Ln3+) doped Bi2O3 nanospheres have been successfully prepared through a solid-state-chemistry thermal decomposition process. The nanospheres exhibit intense upconversion luminescence (UCL) by doping the Ln3+ (Ln = Yb, Er/Ho/Tm) ions into the Bi2O3 host matrix under 980 nm excitation. The ratio of red/green emission of Bi2O3:Yb3+/Er3+ nanospheres exhibits a significant change as the calcination temperature increases and the value could reach 105.6. Moreover, the UCL of Bi2O3:Yb3+/Tm3+ nanospheres are temperature-sensitive, where the intensity ratios of 799 and 808 nm emissions increase monotonously with temperature. The MTT assay reveals that Bi2O3:Yb3+/Tm3+ nanospheres exhibit good biocompatibility by grafting citric acid molecules on the surface. The application possibility of Bi2O3:Yb3+/Tm3+ nanospheres as bioprobes for optical imaging in vivo is also confirmed by the high-contrast photoluminescence images between the background and the UCL imaging area.
Co-reporter:Yanan Li, Liang Zhou, Yunlong Jiang, Rongzhen Cui, Xuesen Zhao, Youxuan Zheng, Jinglin Zuo and Hongjie Zhang
RSC Advances 2016 vol. 6(Issue 68) pp:63200-63205
Publication Date(Web):28 Jun 2016
DOI:10.1039/C6RA14231A
In this work, a series of electroluminescent (EL) devices with single- or double-light-emitting layer(s) (EML) were fabricated to further improve the EL performances of green iridium complex (tfmppy)2Ir(tpip) (tfmppy = 4-trifluoromethylphenylpyridine, tpip = tetraphenylimido-diphosphinate). p-Type material 4,4′,4′′-tri-s(carbazole-9-yl)triphenylamine and bipolar material 2,6-bis(3-(9H-carbazol-9-yl)phenyl)pyridine were chosen as host materials of EML1 and EML2, respectively. Experimental results displayed that not only the doping concentration but also the thicknesses of EML and the electron transport layer strongly influence device performances. Finally, a high performance green EL device with maximum brightness, current efficiency, power efficiency and external quantum efficiency (EQE) up to 113610 cd m−2, 112.30 cd A−1, 97.95 lm W−1 and 29.4%, was realized. Even at the practical brightness of 1000 cd m−2, current efficiency as high as 107.6 cd A−1 (EQE = 28.1%) can still be retained by the same device. To our best knowledge, EL performances of this device were amongst the highest results of the previously reported green devices.
Co-reporter:Yanan Li, Liang Zhou, Rongzhen Cui, Yunlong Jiang, Xuesen Zhao, Weiqiang Liu, Qi Zhu, Yingjie Cui and Hongjie Zhang
RSC Advances 2016 vol. 6(Issue 75) pp:71282-71286
Publication Date(Web):21 Jul 2016
DOI:10.1039/C6RA16517F
In this work, electroluminescent (EL) devices with double light-emitting layers (EMLs) having stepwise energy levels were designed and fabricated to improve the EL performances of the red light-emitting trivalent iridium complex bis(2-methyldibenzo[f,h]quinoxaline)(acetylacetonate)iridium(III) [Ir(MDQ)2(acac)]. To broaden the recombination zone and facilitate the balance of carriers on emitter molecules, the widely used p-type material 4,4′,4′′-tri(N-carbazolyl)triphenylamine (TcTa) and bipolar material 2,6-bis(3-(9H-carbazol-9-yl)phenyl)pyridine (26DCzPPy) were chosen as host materials of EML1 and EML2, respectively due to their well matched energy levels. Interestingly, slight decomposition of Ir(MDQ)2(acac) molecules was observed during the deposition of EML, which causes the rapidly decreased brightness at relatively high doping concentration. Finally, a high performance red EL device with maximum current efficiency of 44.76 cd A−1, power efficiency of 40.19 lm W−1, and external quantum efficiency (EQE) of 15.5% was obtained by optimizing the doping concentration of Ir(MDQ)2(acac). Even at a high brightness of 1000 cd m−2 (5.2 V), a current efficiency as high as 40.59 cd A−1 (EQE = 14.4%) can still be retained by the same device.
Co-reporter:Xia Xu, Peng Zhang, Qinghai Yuan, Pengpeng Lei, Lile Dong, Zhuo Wang, Xiuling Liu, Shuyan Song, Jing Feng and Hongjie Zhang
RSC Advances 2016 vol. 6(Issue 40) pp:33493-33500
Publication Date(Web):22 Mar 2016
DOI:10.1039/C6RA01569G
Rare earth doped upconversion nanoparticles (UCNPs) used as bioprobes for in vivo upconversion luminescence (UCL) deep tissue imaging have been extensively studied. Red emission possesses high penetration length in biological tissue, so it's more convenient for naked eyed red emission to be performed in biological imaging and detection. However, improved in vivo imaging depth based on the NIR-to-red UCL is still challenging and desirable. Herein, novel α-NaYb(Mn)F4:Er3+@NaLuF4 core–shell nanocrystals with enhanced red emission and improved imaging depth have been synthesized. Under 980 nm excitation, there is a 220% increase in red-to-green ratio and even a 400% increase in red-emission when the Yb3+ core doping concentration is increased from 18% to 68% in the core–shell structure. And the UCL signals detection of pork muscle tissues could be visualized even at a depth of 18 mm. By the tail vein injection of PEG modified α-NaYb(Mn)F4:Er3+@NaLuF4 UCNPs, the in vivo and ex vivo NIR-to-red UCL deep tissue imaging present significant UCL signals in liver and spleen. Moreover, the UCNPs could also be used as in vitro and in vivo X-ray computed tomography (CT) contrast agent owing to the large X-ray absorption efficiency and high atomic number of ytterbium and lutetium elements. The synergistic combination of the in vivo NIR-to-red UCL deep tissue and CT imaging could provide comprehensive diagnosis information for cancer.
Co-reporter:L.B. Tong, Q.X. Zhang, Z.H. Jiang, J.B. Zhang, J. Meng, L.R. Cheng, H.J. Zhang
Journal of the Mechanical Behavior of Biomedical Materials 2016 Volume 62() pp:57-70
Publication Date(Web):September 2016
DOI:10.1016/j.jmbbm.2016.04.038
•Ca2Mg6Zn3 is replaced by new Mg–Zn–Ce/La–Ca phase due to Ce/La addition.•Ce/La microalloying increases the yield strength of extruded Mg–Zn–Ca alloy.•Corrosion behavior is accelerated by Ce/La addition.Magnesium alloys are considered as good candidates for biomedical applications, the influence of Ce/La microalloying on the microstructure, mechanical property and corrosion performance of extruded Mg–5.3Zn–0.6Ca (wt%) alloy has been investigated in the current study. After Ce/La addition, the conventional Ca2Mg6Zn3 phases are gradually replaced by new Mg–Zn–Ce/La–(Ca) phases (T1′), which can effectively divide the Ca2Mg6Zn3 phase. The Ca2Mg6Zn3/T1′ structure in Mg–Zn–Ca–0.5Ce/La alloy is favorably broken into small particles during the extrusion, resulting in an obvious refinement of secondary phase. The dynamic recrystallized grain size is dramatically decreased after 0.5Ce/La addition, and the tensile yield strength is improved, while further addition reverses the effect, due to the grain coarsening. However, the corrosion resistance of extruded Mg–Zn–Ca alloy deteriorates after Ce/La addition, because the diameter of secondary phase particle is remarkably decreased, which increases the amount of cathodic sites and accelerates the galvanic corrosion process.
Co-reporter:Xuesen Zhao, Liang Zhou, Yunlong Jiang, Rongzhen Cui, Yanan Li, Youxuan Zheng, Jinglin Zuo, Hongjie Zhang
Organic Electronics 2016 Volume 37() pp:85-92
Publication Date(Web):October 2016
DOI:10.1016/j.orgel.2016.06.025
•Efficient green electroluminescent devices were fabricated.•Blue iridium complexes with wide energy gap were utilized as sensitizers.•Sensitizer molecules within light-emitting layer function as electron trappers.•Sensitizer with lower energy levels has better sensitization effect.In this work, electroluminescent (EL) performances of a green iridium complex (tfmppy)2Ir(tpip) were significantly improved by utilizing wide energy gap iridium complexes FK306 and FIrpic as sensitizers. Due to the low-lying energy levels, the co-doped FK306 or FIrpic molecules function as electron trappers, which are helpful in balancing holes and electrons on (tfmppy)2Ir(tpip) molecules and in broadening exciton recombination zone. Consequently, the co-doped devices displayed high EL efficiencies and slow efficiency roll-off. Compared with FIrpic, FK306 acts as a more effective sensitizer because of its relatively lower energy levels. Consequently, highly efficient green EL device with maximum current efficiency, power efficiency and brightness up to 102.29 cd/A (external quantum efficiency (EQE) of 25.3%), 88.67 lm/W and 96,268 cd/m2, respectively, was realized by optimizing the co-doping concentration of FK306. Even at the practical brightness of 1000 cd/m2, EL current efficiency up to 92.93 cd/A (EQE = 23%) can still be retained.Highly efficient green EL device with maximum current efficiency, power efficiency and brightness up to 102.29 cd/A (external quantum efficiency (EQE) of 25.3%), 88.67 lm/W and 96,268 cd/m2, respectively, was realized by optimizing the co-doping concentration of a wide energy gap blue iridium complex FK306 as sensitizer.
Co-reporter:Liang Zhou, Yunlong Jiang, Rongzhen Cui, Yanan Li, Xuesen Zhao, Ruiping Deng, Hongjie Zhang
Journal of Luminescence 2016 Volume 170(Part 2) pp:692-696
Publication Date(Web):February 2016
DOI:10.1016/j.jlumin.2015.02.053
•Electroluminescent performances of europium complex were further improved.•Device structure with stepwise energy levels was designed.•Better carriers' balance was realized by improving the injection and transport of holes.•The selection of bipolar host caused the broadening of recombination zone.In this study, we aim to further enhance the electroluminescence (EL) performances of trivalent europium complex Eu(TTA)3phen (TTA=thenoyltrifluoroacetone and phen=1,10-phenanthroline) by designing the device structure with stepwise energy levels. The widely used bipolar material 2,6-bis(3-(9H-carbazol-9-yl)phenyl)pyridine (26DCzPPy) was chosen as host material, while the doping concentration of Eu(TTA)3phen was optimized to be 4%. To facilitate the injection and transport of holes, MoO3 anode modification layer and 4,4′,4′′-Tris(carbazole-9-yl)triphenylamine (TcTa) hole transport layer were inserted in sequence. Efficient pure red emission with suppressed efficiency roll-off was obtained attributed to the reduction of accumulation holes, the broadening of recombination zone, and the improved balance of holes and electrons on Eu(TTA)3phen molecules. Finally, the device with 3 nm MoO3 and 5 nm TcTa obtained the highest brightness of 3278 cd/m2, current efficiency of 12.45 cd/A, power efficiency of 11.50 lm/W, and external quantum efficiency of 6.60%. Such a device design strategy helps to improve the EL performances of emitters with low-lying energy levels and provides a chance to simplify device fabrication processes.
Co-reporter:L.B. Tong, J.B. Zhang, Q.X. Zhang, Z.H. Jiang, C. Xu, S. Kamado, D.P. Zhang, J. Meng, L.R. Cheng, H.J. Zhang
Materials Characterization 2016 Volume 115() pp:1-7
Publication Date(Web):May 2016
DOI:10.1016/j.matchar.2016.03.012
•Warm rolling improves the yield strength of extruded alloy.•Basal texture is remarkably enhanced after the rolling.•Twinning and dynamic recrystallization occur during the rolling.Tensile yield strength of extruded Mg–5.3Zn–0.5Ca–0.5Ce/La (weight percent) alloy is remarkably increased to 316 MPa from 163 MPa, via the warm rolling process. The tension twinning can be activated after low-strain (5–21%) rolling, and the dynamic recrystallization occurs with increasing rolling reduction. The dislocations are gradually accumulated within the original grains during the rolling, and the number fraction of low angle grain boundary is increased. The coarse secondary phases are gradually broken into small pieces, due to the increased rolling deformation. The weak fiber texture with 101̅0 parallel to extrusion direction in the extruded alloy is modified to the typical 0002101̅0 texture after rolling, and the yield strength is notably improved, because of the multiple strengthening effects (grain refinement, work hardening, dispersion and texture). A good balance between strength (> 310 MPa) and ductility (~ 9.5%), has been achieved through the warm rolling.
Co-reporter:Xiao Wang, Dapeng Liu, Junqi Li, Jiangman Zhen and Hongjie Zhang
NPG Asia Materials 2015 7(1) pp:e158
Publication Date(Web):2015-01-01
DOI:10.1038/am.2014.128
The fabrication of multi-component hybrid nanostructures is of vital importance because their two-phase interface could provide a rich environment for redox reactions, which are beneficial for enhancing catalytic performance. Inspired by the above consideration, strongly coupled Cu2O@CeO2 core@shell nanostructures have been successfully prepared via a non-organic and clean aqueous route without using any organic additive. In this process, an auto-catalytic redox reaction occurred on the two-phase interface, followed by a triggered self-assembly process. Additionally, the size, morphology and composition of the as-obtained nanostructures can be tuned well by varying the reaction temperature, as well as the species and the amount of Cu precursors. The catalytic tests for peroxidase-like activity and CO oxidation have been conducted in detail, and the results confirm a strong synergistic effect at the interface sites between the CeO2 and Cu2O components.
Co-reporter:Shuyan Song, Xiao Wang and Hongjie Zhang
NPG Asia Materials 2015 7(5) pp:e179
Publication Date(Web):2015-05-01
DOI:10.1038/am.2015.27
Encapsulation of small noble metal nanoparticles has received attention owing to the resulting highly increased stability and high catalytic activity and selectivity. Among the types of inert metal oxides, CeO2 is unique. It is inexpensive and highly stable, and, more importantly, the unique electronic configuration gives it a strong capability to provide active oxygen. The method of fabricating CeO2-encapsulated noble metal nanocatalysts is determined by the requirements of the application. In this review, we first describe the various types of encapsulated noble metals and then the current developments of synthesis in detail, including the types of hybrid nanostructures and successful synthetic strategies. The following section, concerning catalytic applications, is divided into three topics: anti-sintering capabilities, catalytic activities and selectivities. We hope that this review of the recent achievements and the proposed strategy for addressing the emerging challenges will inspire further developments in this research area.
Co-reporter:Xiao Wang, Dapeng Liu, Junqi Li, Jiangman Zhen, Fan Wang and Hongjie Zhang
Chemical Science 2015 vol. 6(Issue 5) pp:2877-2884
Publication Date(Web):27 Feb 2015
DOI:10.1039/C4SC03854A
In this paper, we have successfully demonstrated the clean synthesis of high-quality Pd@CeO2 core@shell nanospheres with tunable Pd core sizes in water, and furthermore loaded the as-obtained Pd@CeO2 products on commercial γ-Al2O3via electrostatic interaction. KBr here plays two key roles in inducing the growth and self-assembly of Pd@CeO2 core@shell nanospheres. First, Br− ions can retard the reduction of Pd2+ ions via the formation of the more stable complex of [PdBr4]2− so as to tune the size of Pd cores. Second, it greatly decreases the colloidal stability, and hence the surface polarity-weakened Pd and CeO2 NPs have to spontaneously self-assemble into more stable and ordered structures. Among different-sized Pd samples, the as-obtained 8 nm-Pd@CeO2/Al2O3 one exhibits the best performance in catalytic CO oxidation, which can catalyze 100% CO conversion into CO2 at 95 °C, which is much lower than the previously reported CeO2-encapsulated Pd samples.
Co-reporter:Shuyan Song, Xiao Wang, Sheling Li, Zhuo Wang, Qi Zhu and Hongjie Zhang
Chemical Science 2015 vol. 6(Issue 11) pp:6420-6424
Publication Date(Web):23 Jul 2015
DOI:10.1039/C5SC01686J
Recent studies have further demonstrated that the conjugation of noble metal helical nanostructures could alter their optical and catalytic activities. However, the intrinsic isotropic crystal growth of Pt makes the synthesis of high-quality Pt NCs with unique porous or branched nanostructures difficult. In this work, a new, powerful capping agent, N,N-dimethyloctadecylammonium bromide acetate sodium, was synthesized and used to coordinate Pt ions, slowing down the reaction rate. As a result, in aqueous solution, Pt nanohelices with highly ordered horizontal pore channels were successfully fabricated. Importantly, the Pt nanohelices were composed of several sub-2 nm Pt nanowires coiled together around a central point. The as-obtained samples exhibited enhanced photothermal properties compared with the classic Pt nanoparticles.
Co-reporter:Zhuo Wang, Peng Zhang, Qinghai Yuan, Xia Xu, Pengpeng Lei, Xiuling Liu, Yue Su, Lile Dong, Jing Feng and Hongjie Zhang
Nanoscale 2015 vol. 7(Issue 42) pp:17861-17870
Publication Date(Web):30 Sep 2015
DOI:10.1039/C5NR04889C
In this paper, intense up- and down-conversion luminescence were successfully achieved in well designed and synthesized core–shell structured NaLuF4:Gd/Yb/Er@NaLuF4:Yb@NaLuF4:Nd/Yb@NaLuF4 nanoparticles (NPs) simultaneously under 808 nm continuous-wave laser excitation. The morphologies, luminescent properties and energy transfer mechanism of the nanoparticles were studied in detail. By employing this design, multimodal imaging performance including near-infrared down-conversion optical imaging and X-ray computed tomography (CT) imaging were realized in one kind of NPs. Furthermore, the 808 nm excited optical temperature sensing property of the synthesized NPs was realized in a wide temperature range by monitoring the intensities of up- and down-conversion luminescence. This study provides a novel platform based on lanthanide fluoride nanoparticles for multifunctional imaging and temperature sensing in one system.
Co-reporter:Xing Meng, Shu-Yan Song, Xue-Zhi Song, Min Zhu, Shu-Na Zhao, Lan-Lan Wu and Hong-Jie Zhang
Chemical Communications 2015 vol. 51(Issue 38) pp:8150-8152
Publication Date(Web):31 Mar 2015
DOI:10.1039/C5CC01732G
A tetranuclear copper cluster-based MOF with sulfonate–carboxylate ligands has been synthesized. It possesses one-dimensional irregular channels lined with sulfonate, carboxylate, and DMF molecules, which show a high proton conductivity of 7.4 × 10−4 S cm−1 at 95 °C and 95% relative humidity.
Co-reporter:Zhiyong Guo, Xuezhi Song, Huaping Lei, Hailong Wang, Shengqun Su, Hui Xu, Guodong Qian, Hongjie Zhang and Banglin Chen
Chemical Communications 2015 vol. 51(Issue 2) pp:376-379
Publication Date(Web):10 Nov 2014
DOI:10.1039/C4CC06729K
A ketone functionalized luminescent terbium metal–organic framework has been realized for the highly selective and sensitive sensing of aniline.
Co-reporter:Liang Zhou, Leijiao Li, Yunlong Jiang, Rongzhen Cui, Yanan Li, Xuesen Zhao, and Hongjie Zhang
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 29) pp:16046
Publication Date(Web):July 15, 2015
DOI:10.1021/acsami.5b04348
In this work, we experimentally demonstrated the new functions of trivalent rare earth complex in improving the electroluminescent (EL) performances of iridium complex by codoping trace Eu(TTA)3phen (TTA = thenoyltrifluoroacetone, phen = 1,10-phenanthroline) into a light-emitting layer based on PQ2Ir(dpm) (iridium(III)bis(2-phenylquinoly-N,C2′)dipivaloylmethane). Compared with a reference device, the codoped devices displayed higher efficiencies, slower efficiency roll-off, higher brightness, and even better color purity. Experimental results demonstrated that Eu(TTA)3phen molecules function as electron trappers due to its low-lying energy levels, which are helpful in balancing holes and electrons and in broadening recombination zone. In addition, the matched triplet energy of Eu(TTA)3phen is instrumental in facilitating energy transfer from host to emitter. Finally, highly efficient red EL devices with the highest current efficiency, power efficiency and brightness up to 58.98 cd A–1 (external quantum efficiency (EQE) of 21%), 61.73 lm W–1 and 100870 cd m–2, respectively, were obtained by appropriately decreasing the doping concentration of iridium complex. At certain brightness of 1000 cd m–2, EL current efficiency up to 51.94 cd A–1 (EQE = 18.5%) was retained. Our investigation extends the application of rare earth complexes in EL devices and provides a chance to improve the device performances.Keywords: carrier trapping; electroluminescence; energy transfer; iridium complex; rare earth complex; recombination zone;
Co-reporter:Pengpeng Lei, Peng Zhang, Qinghai Yuan, Zhuo Wang, Lile Dong, Shuyan Song, Xia Xu, Xiuling Liu, Jing Feng, and Hongjie Zhang
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 47) pp:26346
Publication Date(Web):November 11, 2015
DOI:10.1021/acsami.5b09990
In this work, water-soluble Yb3+/Er3+ codoped Bi2O3 upconversion (UC) nanospheres with uniform morphology have been successfully synthesized via a solid-state-chemistry thermal decomposition process. With 980 nm near-infrared irradiation, the Bi2O3:Yb3+/Er3+ nanospheres have bright UC luminescence (UCL). Moreover, multicolor UC emissions (from green to red) can be tuned by simply changing the Yb3+ ions doping concentration. After citric acid molecules were grafted on the surface of Bi2O3:20% Yb3+/2% Er3+ nanospheres, the MTT assay on HeLa cells and CCK-8 assay on osteoblasts show that the UC nanospheres exhibit excellent stability and biocompatibility. The possibility of using these nanoprobes with red UCL for optical imaging in vivo has been demonstrated. Furthermore, Bi3+ and Yb3+ containing nanospheres as binary contrast agent also exhibited significant enhancement of contrast efficacy than iodine-based contrast agent via X-ray computed tomography (CT) imaging at different voltage setting (80–140 kVp), indicating they have potential as CT imaging contrast agent. Thus, Yb3+/Er3+ codoped Bi2O3 nanospheres could be used as dual modality probe for optical and CT imagings.Keywords: lanthanide; Bi2O3; binary contrast agent; dual-modal imaging; upconversion luminescence
Co-reporter:Xia Xu, Zhuo Wang, Pengpeng Lei, Yingning Yu, Shuang Yao, Shuyan Song, Xiuling Liu, Yue Su, Lile Dong, Jing Feng, and Hongjie Zhang
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 37) pp:20813
Publication Date(Web):August 27, 2015
DOI:10.1021/acsami.5b05876
Novel flower-like α-NaYb(Mn)F4:Er3+/Tm3+@NaYF4 upconversion nanoparticles (UCNPs) as luminescent nanothermometers have been developed by combining liquid–solid solution hydrothermal strategy with thermal decomposition strategy. Under 980 nm excitation, they exhibit intense upconversion luminescence and temperature-dependent upconversion luminescence over a wide temperature range. The influence of temperature on “band-shape” upconversion luminescence (UCL) spectra and the intensity of emission bands are analyzed and discussed in detail. We further successfully test and verify that intensity ratios REr of 2H11/2 → 4I15/2 and 4S3/2 → 4I15/2 and RTm of 1G4 → 3H5 and 3H4 → 3H6 are sensitive to temperature, and the population of active ions follows Boltzmann-type population distribution very well. These luminescent nanothermometers could be applied over a wide temperature range from 123 to 423 K with high sensitivity, which enable them to be excellent candidates for temperature sensors.Keywords: band-shape; lanthanide; luminescent nanothermometer; sensitivity; thermally coupled; upconversion nanoparticles
Co-reporter:Min Zhu;Xue-Zhi Song;Shu-Yan Song;Shu-Na Zhao;Xing Meng;Lan-Lan Wu;Cheng Wang;Hong-Jie Zhang
Advanced Science 2015 Volume 2( Issue 4) pp:
Publication Date(Web):
DOI:10.1002/advs.201500012
Stimuli-responsive structural transformations are emerging as a scaffold to develop a charming class of smart materials. A EuL metal-organic framework (MOF) undergoes a reversible temperature-stimulated single-crystal to single-crystal transformation, showing a specific behavior of fast capture/release of free Eu3+ in the channels at low and room temperatures. At room temperature, compound 1a is obtained with one free carboxylate group severing as further hook, featuring one-dimensional square channels filled with intrinsic free europium ions. Trigged by lowering the ambient temperature, 1b is gained. In 1b, the intrinsic free europium ions can be fast captured by the carboxylate-hooks anchored in the framework, resulting in the structural change and its channel distortion. To the best of our knowledge, this is the first report of such a rapid and reversible switch stemming from dynamic control between noncovalent and covalent Eu–ligand interactions. Utilizing EuL MOF to detect highly explosive 2,4,6-trinitrophenol at room temperature and low temperature provides a glimpse into the potential of this material in fluorescence sensors.
Co-reporter:Fan Wang, Xiao Wang, Dapeng Liu, Jiangman Zhen, Junqi Li and Hongjie Zhang
Dalton Transactions 2015 vol. 44(Issue 48) pp:21124-21130
Publication Date(Web):09 Nov 2015
DOI:10.1039/C5DT03360H
In this work, three kinds of ZnCo2O4 morphologies, that is, rod, plate and sphere, have been successfully prepared and further used to support Pt nanoparticles (NPs) via in situ deposition. The as-prepared ZnCo2O4–Pt hybrid nanomaterials were then carefully characterized by SEM, TEM, XRD, XPS, ICP EDX, and N2 adsorption measurement in great detail. Besides, the three catalysts were also evaluated by the model reaction of catalytic CO oxidation. After comparing the difference in the three kinds of morphologies, we have tried to clarify the reason for their different catalytic performances. As a result, the ZnCo2O4–Pt sphere was found to be the most active, attaining 100% CO conversion at a relatively low temperature of 140 °C, because more Pt NPs are prone to distribution on the surface of ZnCo2O4 spheres than the other ones. The following cycling tests confirm the excellent stability of the as-prepared ZnCo2O4–Pt samples.
Co-reporter:Xia Xu, Zhuo Wang, Pengpeng Lei, Xiuling Liu, Yue Su, Lile Dong, Shuang Yao, Liang Zhou, Shuyan Song, Jing Feng and Hongjie Zhang
Dalton Transactions 2015 vol. 44(Issue 39) pp:17286-17292
Publication Date(Web):2015/09/02
DOI:10.1039/C5DT02751A
Cubic KLu3F10 nanocrystals have been fabricated by doping Mn2+ ions via a liquid–solid solution (LSS) hydrothermal method. With an increase in the Mn2+ level, a phase transformation from orthorhombic KLu2F7 to cubic KLu3F10 associated with evolution of the particle morphologies and sizes is evident. The phase transformation mechanism based on doping with Mn2+ ions was studied via a series of time-controlled experiments and the enhancement of the intensity of upconversion luminescence (UCL) via doping with Mn2+ ions is discussed in detail. In addition, under 980 nm excitation, the UCL properties of Er3+/Tm3+/Ho3+-doped KLu3F10:Yb3+ upconversion nanoparticles (UCNPs) have been investigated and a possible UCL mechanism has been discussed. It has been demonstrated that cubic KLu3F10 is an excellent host for upconversion luminescence.
Co-reporter:Jiangman Zhen, Dapeng Liu, Xiao Wang, Junqi Li, Fan Wang, Yinghui Wang and Hongjie Zhang
Dalton Transactions 2015 vol. 44(Issue 5) pp:2425-2430
Publication Date(Web):15 Dec 2014
DOI:10.1039/C4DT03141E
A fast and facile self-assembly method has been developed to deposit 3–5 nm sized PdxPt1−x (0 ≤ x ≤ 1) nanoparticles (NPs) on Ni(OH)2 nanosheets. The biomolecule L-lysine has been used here as the linker to hybridize PdxPt1−x NPs and Ni(OH)2 nanosheets together. The catalytic properties of the obtained PdxPt1−x/Ni(OH)2 hybrids were evaluated by employing the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) by NaBH4 as a model reaction. The results reveal that the stability, activity and recyclability of PdxPt1−x NPs have been remarkably enhanced after being supported on Ni(OH)2 nanosheets. Moreover, the influence of the composition of noble metals on the catalytic properties has been studied in depth and Pd0.5Pt0.5/Ni(OH)2 hybrids show the optimal catalytic properties.
Co-reporter:Rongzhen Cui, Liang Zhou, Yunlong Jiang, Yanan Li, Xuesen Zhao, Hongjie Zhang
Journal of Luminescence 2015 Volume 166() pp:259-263
Publication Date(Web):October 2015
DOI:10.1016/j.jlumin.2015.05.060
•Yellow electroluminescent devices were designed and fabricated.•P-type and n-type materials having stepwise energy levels were chosen as host materials.•Better balance of holes and electrons causes the enhanced efficiencies.•Improved carriers' trapping suppresses the emission of host material.In this work, we aim to further improve the electroluminescent (EL) performances of a yellow light-emitting iridium(III) complex by designing double light-emitting layers (EMLs) devices having stepwise energy levels. Compared with single-EML devices, these designed double-EML devices showed improved EL efficiency and brightness attributed to better balance in carriers. In addition, the stepwise distribution in energy levels of host materials is instrumental in broadening the recombination zone, thus delaying the roll-off of EL efficiency. Based on the investigation of carriers' distribution, device structure was further optimized by adjusting the thickness of deposited layers. Finally, yellow EL device (Commission Internationale de l'Eclairage (CIE) coordinates of (0.446, 0.542)) with maximum current efficiency, power efficiency and brightness up to 78.62 cd/A (external quantum efficiency (EQE) of 21.1%), 82.28 lm/W and 72,713 cd/m2, respectively, was obtained. Even at the high brightness of 1000 cd/m2, EL efficiency as high as 65.54 cd/A (EQE=17.6%) can be retained.
Co-reporter:Yunlong Jiang, Liang Zhou, Rongzhen Cui, Yanan Li, Xuesen Zhao, Hongjie Zhang
Journal of Luminescence 2015 Volume 168() pp:38-42
Publication Date(Web):December 2015
DOI:10.1016/j.jlumin.2015.07.027
In this work, we report the highly efficient pure blue electroluminescent (EL) device based on bis[(3,5-difluoro-4-cyanophenyl)pyridine]picolinate iridium(III) (FCNIrpic) doped 9-(4-tert-Butylphenyl)-3,6-bis(triphenylsilyl)-9H-carbazole (CzSi) film. The matched energy levels of FCNIrpic and CzSi are helpful in facilitating the trapping of carriers, while the high triplet energy of CzSi can well avoid the undesired reverse energy transfer. More importantly, the injection of holes was further accelerated by inserting 5 nm 4,4′,4″-Tri(9-carbazoyl)triphenylamine (TcTa) film between hole transport layer and lighting-emitting layer (EML) as interlayer. Consequently, EL performances were significantly enhanced attributed to wider recombination zone and better balance of holes and electrons. Interestingly, single-EML device displayed higher performances than those of double-EMLs device. Finally, pure blue EL device with the structure of ITO/MoO3 (3 nm)/TAPC (40 nm)/TcTa (5 nm)/FCNIrpic (20%): CzSi (30 nm)/TmPyPB (40 nm)/LiF (1 nm)/Al (100 nm) realized the maximum brightness, current efficiency, power efficiency and external quantum efficiency up to 12,505 cd/m2, 36.20 cd/A, 28.42 lm/W and 16.9%, respectively. Even at the high brightness of 1000 cd/m2, current efficiency and external quantum efficiency up to 17.40 cd/A and 8.1%, respectively, can be retained by the same device.
Co-reporter:Qingxin ZHANG, Libo TONG, Liren CHENG, Zhonghao JIANG, Jian MENG, Hongjie ZHANG
Journal of Rare Earths 2015 Volume 33(Issue 1) pp:70-76
Publication Date(Web):January 2015
DOI:10.1016/S1002-0721(14)60385-9
The effect of Ce/La misch metal addition on the microstructural evolution of as-cast and as-soluted Mg-5.3Zn-0.5Ca (wt.%) alloys was systematically investigated. It was found that Ce/La could effectively refine the as-cast alloy and restrain grain growth during solution treatment, which was derived from the constitutional supercooling during solidification process and the formation of stable intermetallic compounds CeMg12 and Mg17La2. Furthermore, Ce/La microalloying and solution treatment resulted in an evolution from the original lamellar Ca2Mg6Zn3/α-Mg to the divorced eutectic structure. The thermal stability of Mg-Zn-Ca alloy could be effectively improved by Ce/La addition, because the low-melting-point binary Mg-Zn phase was transformed to MgxZny-Ca-(Ce/La) phase with higher thermal stability and the amount of Ca2Mg6Zn3/α-Mg eutectic structure was reduced.Grain size against solution treatment time curves of Mg-Zn-Ca-xCe/La alloys
Co-reporter:Zhiyong Guo, Shengqun Su, Ruiping Deng, Hongjie Zhang
Inorganic Chemistry Communications 2015 Volume 51() pp:9-12
Publication Date(Web):January 2015
DOI:10.1016/j.inoche.2014.10.030
•Synthesis of a new cobalt-based MOF constructed from a tricarboxylic acid linker.•Compound 1 displays unique (2,3,10)-connected trinodal topology.•Compound 1 represents a rare example of MOF possessing free carboxylic acids.•The magnetic property of compound 1 has been investigated.A 3D metal–organic framework (MOF), [Co3(μ3-OH)(μ2-H2O)(BPT)(HBPT)(DMF)2]·(DMF)(H2O) (1) (DMF = N, N′-dimethylformamide) has been synthesized by self-assembly of cobalt(II) oxide and biphenyl-3, 4′, 5-tricarboxylate (H3BPT) under solvothermal reaction. Compound 1 displays unique (2,3,10)-connected trinodal connected topology. Besides, 1 represents a rare example of MOF possessing free carboxylic acids. In addition, the magnetic property of the compound is investigated.A novel cobalt based MOF with intriguing topology has been synthesized and characterized by various state-of-the-art methods. It represents a rare example of MOF containing free carboxylic acids. In addition, the magnetic property of the compound is investigated.
Co-reporter:Jiangman Zhen;Xiao Wang;Dapeng Liu;Zhuo Wang;Junqi Li;Fan Wang
Nano Research 2015 Volume 8( Issue 6) pp:1944-1955
Publication Date(Web):2015 June
DOI:10.1007/s12274-015-0704-3
In this study, Co3O4@CeO2 core@shell nanowires were successfully prepared via thermal decomposition of Co(CO3)0.5(OH)·0.11H2O@CeO2 core@shell nanowire precursors. As a CO oxidation catalyst, Co3O4@CeO2 shows remarkably enhanced catalytic performance compared to Co3O4 nanowires and CeO2 nanoparticles (NPs), indicating obvious synergistic effects between the two components. It also suggests that the CeO2 shell coating can effectively prevent Co3O4 nanowires from agglomerating, hence effecting a substantial improvement in the structural stability of the Co3O4 catalyst. Furthermore, the fabrication of the well-dispersed core@shell structure results in a maximized interface area between Co3O4 and CeO2, as well as a reduced Co3O4 size, which may be responsible for the enhanced catalytic activity of Co3O4@CeO2. Further examination revealed that CO oxidation may occur at the interface of Co3O4 and CeO2. The influence of calcination temperatures and the component ratio between Co3O4 and CeO2 were then investigated in detail to determine the catalytic performance of Co3O4@CeO2 core@shell nanowires, the best of which was obtained by calcination at 250 °C for 3 h with a Ce molar concentration of about 38.5%. This sample achieved 100% CO conversion at a reduced temperature of 160 °C. More importantly, more than 2.5 g of the Co3O4@CeO2 core@shell nanowires were produced in one pot by this simple process, which may be beneficial for practical applications as automobile-exhaust gas-treatment catalysts.
Co-reporter:Song Dang;Shuyan Song;Jing Feng;Hongjie Zhang
Science China Chemistry 2015 Volume 58( Issue 6) pp:973-978
Publication Date(Web):2015 June
DOI:10.1007/s11426-014-5272-y
Nanoscale europium(III) metal-organic frameworks, Eu(BTC)(H2O)·DMF, were synthesized by rapid microwave-assisted method. The components of the as-prepared products were confirmed by the elemental analysis, X-ray powder diffraction (XRD), thermal gravimetric analysis (TGA) and Fourier-transform infrared spectra (FTIR) analyses. Eu(BTC)(H2O)·DMF with various morphologies, including particle-like, rod-like, straw-sheaf-like nanostructures, could be simply prepared by controlling the concentrations of the starting reactants. The optical measurements on the obtained Eu(BTC)(H2O)·DMF indicated that all the nanomaterials show the characteristic emissions of the Eu3+ ions at 578, 590, 612, 650, and 699 nm, which were attributed to 5D0→7FJ (J=0–4) transitions of the Eu3+ ion, respectively. It was also noticed that the luminescent properties of the as-prepared products were heavily dependent on the morphologies and sizes of the nanomaterials. The assembled straw-sheaf-like architectures displayed the strongest emissions and the longest luminescence lifetime, which was mainly due to the fewest surface defects.
Co-reporter:L.B. Tong, M.Y. Zheng, S. Kamado, D.P. Zhang, J. Meng, L.R. Cheng, H.J. Zhang
Journal of Magnesium and Alloys 2015 Volume 3(Issue 4) pp:302-308
Publication Date(Web):December 2015
DOI:10.1016/j.jma.2015.08.007
The influence of equal channel angular pressing on the tension–compression yield asymmetry of extruded Mg–5.3 Zn–0.6 Ca (weight percent) alloy has been investigated. The microstructure was obviously refined by the large strain during the equal channel angular pressing, accompanied with very fine Ca2Mg6Zn3 phases with average diameter of 70 nm. The weak tension–compression yield asymmetry after equal channel angular pressing is mainly attributed to the reduced volume fraction of extension twinning during the compression, because the slope (k) of twinning in Hall–Petch relationship is higher than that of dislocation slip, and the twinning deformation is difficult to take place with decreasing grain size. The basal slip is more active in the alloy after equal channel angular pressing, due to the non-basal texture components, which hinders the twinning activation and reduces the yield asymmetry. Furthermore, the presence of fine precipitate restricts the twinning activation, which also contributes to the reduction of yield asymmetry.
Co-reporter:L.B. Tong, Q.X. Zhang, Z.H. Jiang, J. Meng, H.J. Zhang
Materials Science and Engineering: A 2015 620() pp: 483-489
Publication Date(Web):
DOI:10.1016/j.msea.2014.10.005
Co-reporter:L.B. Tong, M.Y. Zheng, L.R. Cheng, D.P. Zhang, S. Kamado, J. Meng, H.J. Zhang
Materials Characterization 2015 104() pp: 66-72
Publication Date(Web):
DOI:10.1016/j.matchar.2014.09.020
Co-reporter:Yinghui Wang;Shuyan Song;Jianhua Liu;Dapeng Liu; Hongjie Zhang
Angewandte Chemie International Edition 2015 Volume 54( Issue 2) pp:536-540
Publication Date(Web):
DOI:10.1002/anie.201409519
Abstract
Limited therapeutic efficiency and severe side effects in patients are two major issues existing in current chemotherapy of cancers in clinic. To design a proper theranostic platform seems thus quite needed to target cancer cells accurately by bioimaging and simultaneously release drugs on demand without premature leakage. A novel ZnO-functionalized upconverting nanotheranostic platform has been fabricated for clear multi-modality bioimaging (upconversion luminescence (UCL), computed tomography (CT), and magnetic resonance imaging (MRI)) and specific pH-triggered on-demand drug release. In our theranostic platform multi-modality imaging provides much more detailed and exact information for cancer diagnosis than single-modality imaging. In addition, ZnO can play the role of a “gatekeeper” to efficiently block the drug in the mesopores of the as-prepared agents until it is dissolved in the acidic environment around tumors to realize sustained release of the drug. More importantly, the biodegradable ZnO, which is non-toxic against normal tissues, endows the as-prepared agents with high therapeutic effectiveness but very low side effects. These findings are of great interests and will inspire us much to develop novel effective imaging-guided on-demand chemotherapies in cancer treatment.
Co-reporter:Dr. Xiyan Li;Xiaowang Liu;Daniel M. Chevrier;Dr. Xian Qin;Dr. Xiaoji Xie;Dr. Shuyan Song; Hongjie Zhang; Peng Zhang; Xiaogang Liu
Angewandte Chemie International Edition 2015 Volume 54( Issue 45) pp:13312-13317
Publication Date(Web):
DOI:10.1002/anie.201507176
Abstract
We report the synthesis and characterization of cubic NaGdF4:Yb/Tm@NaGdF4:Mn core–shell structures. By taking advantage of energy transfer through YbTmGdMn in these core–shell nanoparticles, we have realized upconversion emission of Mn2+ at room temperature in lanthanide tetrafluoride based host lattices. The upconverted Mn2+emission, enabled by trapping the excitation energy through a Gd3+ lattice, was validated by the observation of a decreased lifetime from 941 to 532 μs in the emission of Gd3+ at 310 nm (6P7/28S7/2). This multiphoton upconversion process can be further enhanced under pulsed laser excitation at high power densities. Both experimental and theoretical studies provide evidence for Mn2+ doping in the lanthanide-based host lattice arising from the formation of F− vacancies around Mn2+ ions to maintain charge neutrality in the shell layer.
Co-reporter:Dr. Xiyan Li;Xiaowang Liu;Daniel M. Chevrier;Dr. Xian Qin;Dr. Xiaoji Xie;Dr. Shuyan Song; Hongjie Zhang; Peng Zhang; Xiaogang Liu
Angewandte Chemie 2015 Volume 127( Issue 45) pp:13510-13515
Publication Date(Web):
DOI:10.1002/ange.201507176
Abstract
We report the synthesis and characterization of cubic NaGdF4:Yb/Tm@NaGdF4:Mn core–shell structures. By taking advantage of energy transfer through YbTmGdMn in these core–shell nanoparticles, we have realized upconversion emission of Mn2+ at room temperature in lanthanide tetrafluoride based host lattices. The upconverted Mn2+emission, enabled by trapping the excitation energy through a Gd3+ lattice, was validated by the observation of a decreased lifetime from 941 to 532 μs in the emission of Gd3+ at 310 nm (6P7/28S7/2). This multiphoton upconversion process can be further enhanced under pulsed laser excitation at high power densities. Both experimental and theoretical studies provide evidence for Mn2+ doping in the lanthanide-based host lattice arising from the formation of F− vacancies around Mn2+ ions to maintain charge neutrality in the shell layer.
Co-reporter:Xue-Zhi Song;Shu-Yan Song;Shu-Na Zhao;Zhao-Min Hao;Min Zhu;Xing Meng;Lan-Lan Wu;Hong-Jie Zhang
Advanced Functional Materials 2014 Volume 24( Issue 26) pp:4034-4041
Publication Date(Web):
DOI:10.1002/adfm.201303986
A sensor with a red-emission signal is successfully obtained by the solvothermal reaction of Eu3+ and heterofunctional ligand bpydbH2 (4,4′-(4,4′-bipyridine-2,6-diyl) dibenzoic acid), followed by terminal-ligand exchange in a single-crystal-to-single-crystal transformation. As a result of treatments both before and after the metal–organic framework formation, accessible Lewis-base sites and coordinated water molecules are successfully anchored onto the host material, and they act as signal transmission media for the recognition of analytes at the molecular level. This is the first reported sensor based on a metal–organic framework (MOF) with multi-responsive optical sensing properties. It is capable of sensing small organic molecules and inorganic ions, and unprecedentedly it can discriminate among the homologues and isomers of aliphatic alcohols as well as detect highly explosive 2,4,6-trinitrophenol (TNP) in water or in the vapor phase. This work highlights the practical application of luminescent MOFs as sensors, and it paves the way toward other multi-responsive sensors by demonstrating the incorporation of various functional groups into a single framework.
Co-reporter:Zhuo Wang, Jing Feng, Shuyan Song, Zhiqiang Sun, Shuang Yao, Xin Ge, Min Pang and Hongjie Zhang
Journal of Materials Chemistry A 2014 vol. 2(Issue 42) pp:9004-9011
Publication Date(Web):08 Sep 2014
DOI:10.1039/C4TC01778A
The pure and intense orange upconversion luminescence of Eu3+ was efficiently achieved in NaYF4 and NaLuF4 nanocrystals through the upconversion sensitization of doped Yb3+ and Mn2+ ions dimer for the first time. A shell-coating strategy was performed to further enhance the emission intensity. In this work, a novel upconversion mechanism for energy transfer from the Yb3+–Mn2+ dimer to the Eu3+ ion was proposed by analyzing the upconversion luminescence spectra, lifetimes and pumping photons measurements of the obtained nanocrystals in detail. The applications of the nanocrystals for CT imaging and ratiometric pH sensing in physiological pH range were performed. This study also provides a new upconversion spectral region at around 592 nm for applications in multicolor imaging, multiplexed encoding and detection.
Co-reporter:Min Zhu, Zhao-Min Hao, Xue-Zhi Song, Xing Meng, Shu-Na Zhao, Shu-Yan Song and Hong-Jie Zhang
Chemical Communications 2014 vol. 50(Issue 15) pp:1912-1914
Publication Date(Web):13 Dec 2013
DOI:10.1039/C3CC48764D
A new type of 3D lanthanide(III) metal–organic framework directly constructed by double-chain motifs was synthesized. It shows a proton conductivity of 1.6 × 10−5 S cm−1 at 75 °C at 97% RH, and tunable emission including white light.
Co-reporter:Fan Wang, Xiao Wang, Dapeng Liu, Jiangman Zhen, Junqi Li, Yinghui Wang, and Hongjie Zhang
ACS Applied Materials & Interfaces 2014 Volume 6(Issue 24) pp:22216
Publication Date(Web):November 21, 2014
DOI:10.1021/am505853p
In this paper, we report a self-assembly method to synthesize high-quality ZnCo2O4@CeO2 core@shell microspheres with tunable CeO2 thickness. ZnCo2O4 spheres were first synthesized as the core, followed by a controlled CeO2 shell coating process. The thickness of CeO2 shell could be easily tuned by varying the feeding molar ratio of Ce/Co. Transmission electron microscope (TEM) images and scanning transmission electron microscope (STEM) image have identified the core@shell structure of these samples. In CO oxidation tests these ZnCo2O4@CeO2 core@shell microspheres exhibited promising catalytic performance, and the catalytic activity of the best sample is even close to the traditional noble metal-CeO2 system, attaining 100% CO conversion at a relatively low temperature of 200 °C. Cycling tests confirm their good stability of these core@shell microspheres besides activity. Their high catalytic performance should be attributed to the core@shell structure formation, and moreover further H2–temperature-programmed reduction (TPR) results revealed the possible synergistic effects between the two components of ZnCo2O4 and CeO2.Keywords: CeO2; CO oxidation; core@shell; microspheres; ZnCo2O4
Co-reporter:Xing Meng, Rong-Lin Zhong, Xue-Zhi Song, Shu-Yan Song, Zhao-Min Hao, Min Zhu, Shu-Na Zhao and Hong-Jie Zhang
Chemical Communications 2014 vol. 50(Issue 48) pp:6406-6408
Publication Date(Web):16 Apr 2014
DOI:10.1039/C4CC00553H
A 3D pillar-layer framework (1) with uncoordinated carboxyl groups exhibits exceptional stability. It can effectively and selectively adsorb Cu2+ ions and has been applied as a chromatographic column for separating Cu2+/Co2+ ions.
Co-reporter:Xiyan Li, Dapeng Liu, Shuyan Song, and Hongjie Zhang
Crystal Growth & Design 2014 Volume 14(Issue 11) pp:5506-5511
Publication Date(Web):October 9, 2014
DOI:10.1021/cg501164c
Magnetic composite microspheres consisting of a SiO2-coated Fe3O4 core, an ordered TiO2 hierarchically structured shell, and a Pt nanoparticle layer dispersed on the surface of the TiO2 nanoplatelets have been successfully synthesized using a facile and efficient method. The shells of TiO2 hierarchical microspheres were assembled from nanoplatelets, which exposed the high-energy {001} facets, and the Pt nanoparticles were evenly deposited on the surface of the TiO2 nanoplatelets, with a concentration of ∼1 wt %. The resulting composite microspheres exhibited flower-like hierarchical structures with a 202.42 m2 g–1 surface area and possessed superparamagnetic properties with a high saturation magnetization of 31.5 emu g–1. These features endow the obtained composite microspheres with a high adsorption capacity and strong magnetic responsivity that could be easily separated by an external magnetic field. The high photocatalytic activity toward Rhodamine B (RhB) degradation may be caused by the hierarchically structured TiO2 with exposed high-energy {001} facets and the Pt nanoparticle deposits on TiO2 surfaces, which would be efficient for the electron transfer reactions. In addition, the composite microspheres showed high recycling efficiency and stability over several separation cycles.
Co-reporter:Song Wang, Jing Feng, Shuyan Song and Hongjie Zhang
RSC Advances 2014 vol. 4(Issue 99) pp:55897-55899
Publication Date(Web):17 Oct 2014
DOI:10.1039/C4RA09686J
A long-wave optical pH sensor based on intense red upconversion (UC) luminescence of NaGdF4 nanotubes and bromothymol blue was explored. By detecting the UC spectra of NaGdF4 nanotubes in aqueous solution, the sensing system could work on the pH measurement. The intensities of the red emission were linear with pH value changing from 6 to 8.
Co-reporter:L.B. Tong, X. Li, D.P. Zhang, L.R. Cheng, J. Meng, H.J. Zhang
Materials Characterization 2014 92() pp: 77-83
Publication Date(Web):
DOI:10.1016/j.matchar.2014.03.006
Co-reporter:Jiangman Zhen;Xiao Wang;Dr. Dapeng Liu;Dr. Shuyan Song;Zhuo Wang;Dr. Yinghui Wang;Junqi Li;Fan Wang; Hongjie Zhang
Chemistry - A European Journal 2014 Volume 20( Issue 15) pp:4469-4473
Publication Date(Web):
DOI:10.1002/chem.201304109
Abstract
Mastery of nanomaterial structure enables the control of its properties to enhance its performance for a given application. Herein, we demonstrate a fast and facile self-assembly method for the synthesis of a series of Co3O4@CeO2 core@shell cubes, which are characterized by SEM, TEM, XRD, inductively coupled plasma mass spectrometry (ICP-MS), and X-ray photoelectron spectroscopy (XPS) analyses. The results indicate that the thickness of the CeO2 shell can be tuned through simple variation of the feeding molar ratio of Ce/Co. These Co3O4@CeO2 core@shell cubes are used for catalytic CO oxidation and show good catalytic properties. Moreover, the relationship between the catalytic performance and the CeO2 shell thickness is studied in depth to optimize the catalytic properties.
Co-reporter:Xiao Wang ; Dapeng Liu ; Shuyan Song ;Hongjie Zhang
Journal of the American Chemical Society 2013 Volume 135(Issue 42) pp:15864-15872
Publication Date(Web):September 29, 2013
DOI:10.1021/ja4069134
A clean nonorganic synthetic method has been developed to fabricate the uniform pomegranate-like Pt@CeO2 multicore@shell nanospheres in a large scale. Under the effective protection of Ar atmosphere the redox reaction just simply happened between Ce(NO3)3 and K2PtCl4 in an alkaline aqueous solution, in which no other reducing agents or surfactants were added. The as-obtained nanospheres exhibited excellent structure stability even being calcined at 600 °C for 5 h. Moreover, the as-obtained Pt@CeO2 multicore@shell nanospheres can be further supported on reduced graphene oxide (RGO) to form heterogeneous nanocatalyst, which has been successfully applied in the chemical reduction reaction of nitrophenol (NP) by ammonia borane (NH3BH3, dubbed as AB) instead of hazardous H2 or NaBH4.
Co-reporter:Xing Meng, Xue-Zhi Song, Shu-Yan Song, Guo-Cheng Yang, Min Zhu, Zhao-Min Hao, Shu-Na Zhao and Hong-Jie Zhang
Chemical Communications 2013 vol. 49(Issue 76) pp:8483-8485
Publication Date(Web):16 Jul 2013
DOI:10.1039/C3CC44106G
3D pillar-layer framework 1 with [24-MC-6] heterometallic crown clusters exhibits proton conductivity and selective sensing of acetone as well as Cu2+ ions.
Co-reporter:Shunhao Pan, Ruiping Deng, Jing Feng, Shuyan Song, Song Wang, Min Zhu and Hongjie Zhang
CrystEngComm 2013 vol. 15(Issue 38) pp:7640-7643
Publication Date(Web):22 Aug 2013
DOI:10.1039/C3CE40961A
Hydrophilic BaYF5 nanocrystals have been prepared via a facile and fast microwave-assisted method at low temperature without the assistance of template reagents. The Yb3+/Er3+, Ce3+/Tb3+ doped BaYF5 nanocrystals could be dispersed well in water and alcohol. BaYF5:Ce3+/Tb3+ nanocrystals show bright green luminescence. The existence of the Ce3+ ions can dramatically enhance the luminescence intensity of the Tb3+ ions, due to the efficient energy transfer from Ce3+ to Tb3+ ions. More importantly, when doped with Yb3+/Er3+ ions, the BaYF5 nanocrystals show bright red upconversion luminescence.
Co-reporter:Xue-Zhi Song, Shu-Yan Song, Min Zhu, Zhao-Min Hao, Xing Meng, Shu-Na Zhao and Hong-Jie Zhang
Dalton Transactions 2013 vol. 42(Issue 36) pp:13231-13240
Publication Date(Web):21 Jun 2013
DOI:10.1039/C3DT51241J
Hydrothermal reaction of a tripodal bridging ligand, 5-(4-carboxyphenoxy)isophthalic acid (H3cpia) with cobalt salts modulated by N-donor neutral ligands leads to the formation of six novel coordination networks formulated as {[Co1.5(cpia)(o-bix)](H2O)1.5}n (1), {[Co2(cpia)(μ-OH)(m-bix)]H2O}n (2), {[Co1.5(cpia)(m-bix)]}n (3), {[Co1.5(cpia)(p-bix)0.5(H2O)]H2O}n (4), {[Co2.5(cpia)(Hcpia)(4,4′-bpy)2.5](H2O)3}n (5), and {[Co3(cpia)2(bpp)2]H2O}n (6). Compound 1 exhibits a two-dimensional, (3,8)-connected layered architecture composed of trinuclear cobalt clusters. Compound 2 possesses a three-dimensional dense framework with (3,8)-connected tfz-d topology built from butterfly-shaped tetranuclear Co4(μ3-OH)26+ clusters. Similar to compound 1, trinuclear Co clusters act as secondary building units to construct the final 2D layered structure modulated by m-bix and bpp ligands in compounds 3 and 6. In compound 4, trinuclear Co clusters connected by cpia3− anions give rise to two-dimensional layers, which are further pillared by p-bix ligands to the three-dimensional framework. Compound 5 features a 2D, (3,4,6)-connected molecular network assembled from alternate binuclear and mononuclear Co building blocks. The magnetic investigation indicates that strong antiferromagnetic interactions between cobalt ions are dominant in compounds 2 and 6.
Co-reporter:Yunlong Jiang, Liang Zhou, Rongzhen Cui, Yanan Li, Xuesen Zhao, Hongjie Zhang
Journal of Luminescence (December 2015) Volume 168() pp:38-42
Publication Date(Web):1 December 2015
DOI:10.1016/j.jlumin.2015.07.027
In this work, we report the highly efficient pure blue electroluminescent (EL) device based on bis[(3,5-difluoro-4-cyanophenyl)pyridine]picolinate iridium(III) (FCNIrpic) doped 9-(4-tert-Butylphenyl)-3,6-bis(triphenylsilyl)-9H-carbazole (CzSi) film. The matched energy levels of FCNIrpic and CzSi are helpful in facilitating the trapping of carriers, while the high triplet energy of CzSi can well avoid the undesired reverse energy transfer. More importantly, the injection of holes was further accelerated by inserting 5 nm 4,4′,4″-Tri(9-carbazoyl)triphenylamine (TcTa) film between hole transport layer and lighting-emitting layer (EML) as interlayer. Consequently, EL performances were significantly enhanced attributed to wider recombination zone and better balance of holes and electrons. Interestingly, single-EML device displayed higher performances than those of double-EMLs device. Finally, pure blue EL device with the structure of ITO/MoO3 (3 nm)/TAPC (40 nm)/TcTa (5 nm)/FCNIrpic (20%): CzSi (30 nm)/TmPyPB (40 nm)/LiF (1 nm)/Al (100 nm) realized the maximum brightness, current efficiency, power efficiency and external quantum efficiency up to 12,505 cd/m2, 36.20 cd/A, 28.42 lm/W and 16.9%, respectively. Even at the high brightness of 1000 cd/m2, current efficiency and external quantum efficiency up to 17.40 cd/A and 8.1%, respectively, can be retained by the same device.
Co-reporter:Shu-Na Zhao, Xue-Zhi Song, Shu-Yan Song, Hong-jie Zhang
Coordination Chemistry Reviews (15 April 2017) Volume 337() pp:
Publication Date(Web):15 April 2017
DOI:10.1016/j.ccr.2017.02.010
•MOFs can decompose to nanocomposites for heterogeneous catalysis via calcination.•The advantages of MOF-derived nanomaterials can improve catalysis activities.•MOFs can use as excellent supports for catalytic active species.Metal-organic frameworks (MOFs), as novel developing porous crystalline materials, are promising candidates in the field of heterogeneous catalysis because of their high surface area, diverse structures, low densities, adjusted pore sizes, etc. Recently, increasing attention has focused on developing MOF-supported/derived materials as heterogeneous catalysts. In this review, we present the recent development of MOFs as supports or precursors in the preparation of various functional nanomaterials for heterogeneous catalytic reactions including electrocatalysis, organocatalysis, and photocatalysis. Here, we present a comprehensive discussion on the recent progress and the rational design of MOF-supported or derived heterogeneous catalysts to provide insights into the future development of novel and highly efficient heterogeneous catalysts.In this review, we have taken into consideration of the most recent progress and presented comprehensive investigation, discussion and challenges of rational design MOF-supported or derived heterogeneous catalysts for electrocatalysis, organocatalysis, photocatalysis.
Co-reporter:Yanan Li, Liang Zhou, Yunlong Jiang, Rongzhen Cui, Xuesen Zhao and Hongjie Zhang
Journal of Materials Chemistry A 2017 - vol. 5(Issue 17) pp:NaN4225-4225
Publication Date(Web):2017/03/28
DOI:10.1039/C7TC00725F
In this work, we demonstrated a novel device design strategy to obtain efficient pure blue organic fluorescent electroluminescent (EL) devices by doping a traditional electron transport material, 9,10-bis[4-(6-methylbenzothiazol-2-yl)phenyl]anthracene (DBzA), into a hole transporting host material, 4,4′,4′′-tris(carbazol-9-yl)-triphenylamine (TcTa), as the light-emitting layer (EML). Here, DBzA functions not only as a blue emitter but also as an electron transport material. Due to the well matched energy levels of DBzA and TcTa, the obtained devices displayed a broadened recombination zone, improved trapping of carriers, and balanced distribution of holes and electrons on emitter molecules. Interestingly, a single-EML device displayed higher EL efficiencies and lower operation voltage than those of a double-EML device. Finally, a pure blue EL device (Commission Internationale de l'Eclairage (CIE) coordinates of (0.141, 0.165)) with maximum brightness, current efficiency, power efficiency and external quantum efficiency (EQE) of up to 10384 cd m−2, 6.41 cd A−1, 6.71 lm W−1, and 4.3%, respectively, was realized by optimizing the doping concentration. Even at a certain brightness of 1000 cd m−2, current efficiency as high as 4.1 cd A−1 (EQE = 2.8%) can be retained by the same device.
Co-reporter:Rongzhen Cui, Weiqiang Liu, Liang Zhou, Xuesen Zhao, Yunlong Jiang, Youxuan Zheng and Hongjie Zhang
Journal of Materials Chemistry A 2017 - vol. 5(Issue 8) pp:NaN2073-2073
Publication Date(Web):2017/01/24
DOI:10.1039/C6TC05542G
In this work, we demonstrated the efficacy and feasibility of utilizing terbium and gadolinium complexes with low-lying energy levels to sensitize red-emitting iridium complexes in organic light-emitting diodes (OLEDs). Compared with devices without the introduction of a sensitizer, the obtained sensitized devices showed remarkably enhanced electroluminescence performances, which can be attributed to improved carrier balance as well as a wider recombination zone. Moreover, characteristic sensitizer emission was invisible in all sensitized devices due to the inferior hole trapping ability of sensitizer molecules. Finally, the sensitized device co-doped with 0.4 wt% of the terbium complex realized superior electroluminescence performances with maximum brightness, current efficiency, power efficiency and external quantum efficiency as high as 145071 cd m−2, 64.87 cd A−1, 69.11 lm W−1 and 24.7%, respectively. Meanwhile, even at the practical brightness of 1000 cd m−2 (4.0 V), outstanding external quantum efficiency and current efficiency up to 22.7% and 59.7 cd A−1, respectively, were obtained.
Co-reporter:Xing Meng, Hai-Ning Wang, Shu-Yan Song and Hong-Jie Zhang
Chemical Society Reviews 2017 - vol. 46(Issue 2) pp:NaN480-480
Publication Date(Web):2016/12/05
DOI:10.1039/C6CS00528D
Crystalline porous materials are currently a hot research topic in the field of proton-conducting materials. Crystalline porous materials include metal–organic frameworks (MOFs), coordination polymers (CPs), polyoxometalates (POMs) and covalent organic frameworks (COFs). The designable structures and high surface areas of these materials provide great opportunities to orderly accommodate proton carriers and to systemically modify the concentration and mobility of proton carriers in available spaces. Based on the understanding of the relationship between the structure and proton conductivity, controllable synthesis of porous materials with high proton conductivity will gradually be achieved. This review summarizes the emerging studies of these materials and their unique proton conductivities.
Co-reporter:Xing Meng, Shu-Yan Song, Xue-Zhi Song, Min Zhu, Shu-Na Zhao, Lan-Lan Wu and Hong-Jie Zhang
Chemical Communications 2015 - vol. 51(Issue 38) pp:NaN8152-8152
Publication Date(Web):2015/03/31
DOI:10.1039/C5CC01732G
A tetranuclear copper cluster-based MOF with sulfonate–carboxylate ligands has been synthesized. It possesses one-dimensional irregular channels lined with sulfonate, carboxylate, and DMF molecules, which show a high proton conductivity of 7.4 × 10−4 S cm−1 at 95 °C and 95% relative humidity.
Co-reporter:Min Zhu, Zhao-Min Hao, Xue-Zhi Song, Xing Meng, Shu-Na Zhao, Shu-Yan Song and Hong-Jie Zhang
Chemical Communications 2014 - vol. 50(Issue 15) pp:NaN1914-1914
Publication Date(Web):2013/12/13
DOI:10.1039/C3CC48764D
A new type of 3D lanthanide(III) metal–organic framework directly constructed by double-chain motifs was synthesized. It shows a proton conductivity of 1.6 × 10−5 S cm−1 at 75 °C at 97% RH, and tunable emission including white light.
Co-reporter:Xing Meng, Rong-Lin Zhong, Xue-Zhi Song, Shu-Yan Song, Zhao-Min Hao, Min Zhu, Shu-Na Zhao and Hong-Jie Zhang
Chemical Communications 2014 - vol. 50(Issue 48) pp:NaN6408-6408
Publication Date(Web):2014/04/16
DOI:10.1039/C4CC00553H
A 3D pillar-layer framework (1) with uncoordinated carboxyl groups exhibits exceptional stability. It can effectively and selectively adsorb Cu2+ ions and has been applied as a chromatographic column for separating Cu2+/Co2+ ions.
Co-reporter:Xiao Wang;Shuna Zhao;Yibo Zhang;Zhuo Wang;Jing Feng;Shuyan Song;Hongjie Zhang
Chemical Science (2010-Present) 2016 - vol. 7(Issue 2) pp:NaN1114-1114
Publication Date(Web):2016/01/26
DOI:10.1039/C5SC03430B
Recently, mixed metal oxides have attracted tremendous interest because of their great importance for fundamental studies and practical applications in the catalytic field to replace expensive noble metals. Herein, we report the designed synthesis of novel CeO2–Co3O4 mixed metal oxides with complex nanostructures using uniform short CeO2 nanowires self-inserted into ZIF-67 nanocrystals as precursors followed by a thermal annealing treatment. Interestingly, such a synthetic strategy can be easily extended to fabricate other CeO2 nanowires inserted into metal oxide nanoframeworks such as NiCo2O4 and ZnCo2O4. Choosing the NO reduction reaction by CO as the catalytic model, the as-obtained CeO2–Co3O4 hybrids exhibited enhanced catalytic performance, which could be attributed to the strong two-phase interaction between each component.
Co-reporter:Xiao Wang, Dapeng Liu, Junqi Li, Jiangman Zhen, Fan Wang and Hongjie Zhang
Chemical Science (2010-Present) 2015 - vol. 6(Issue 5) pp:NaN2884-2884
Publication Date(Web):2015/02/27
DOI:10.1039/C4SC03854A
In this paper, we have successfully demonstrated the clean synthesis of high-quality Pd@CeO2 core@shell nanospheres with tunable Pd core sizes in water, and furthermore loaded the as-obtained Pd@CeO2 products on commercial γ-Al2O3via electrostatic interaction. KBr here plays two key roles in inducing the growth and self-assembly of Pd@CeO2 core@shell nanospheres. First, Br− ions can retard the reduction of Pd2+ ions via the formation of the more stable complex of [PdBr4]2− so as to tune the size of Pd cores. Second, it greatly decreases the colloidal stability, and hence the surface polarity-weakened Pd and CeO2 NPs have to spontaneously self-assemble into more stable and ordered structures. Among different-sized Pd samples, the as-obtained 8 nm-Pd@CeO2/Al2O3 one exhibits the best performance in catalytic CO oxidation, which can catalyze 100% CO conversion into CO2 at 95 °C, which is much lower than the previously reported CeO2-encapsulated Pd samples.
Co-reporter:Xia Xu, Pengpeng Lei, Lile Dong, Xiuling Liu, Yue Su, Shuyan Song, Jing Feng and Hongjie Zhang
Dalton Transactions 2016 - vol. 45(Issue 20) pp:NaN8446-8446
Publication Date(Web):2016/04/15
DOI:10.1039/C6DT00707D
Controlling excitation and emission wavelengths on demand is very significant in bioimaging. Up-conversion nanoparticles (UCNPs) emit visible light upon near-infrared (NIR) light excitation and are well studied in bioimaging. Red emission is usually preferred to green due to its higher tissue penetration depth in bioimaging. Herein, dominant red emission has been achieved under 808 nm excitation based on the designed α-NaYbF4:Mn2+/Er3+@NaLuF4:Mn2+/Yb3+@NaNdF4:Yb3+@NaGdF4 (C@S1@S2@S3) nanostructure. The rationally designed interlayer shell NaLuF4:Mn2+/Yb3+ could efficiently filter unwanted energy back-transfer from Er3+ to Nd3+ and the outmost shell NaGdF4 could prevent excitation energy from surface-related quenching. The lifetime of 4F9/2 → 4I15/2 transition of Er3+ could be as high as 0.7 ms. Moreover, C@S1@S2@S3 UCNPs also possess effective contrast efficiency for both X-ray computed tomography (CT) and magnetic resonance (MR) imaging. The designed multifunctional UCNPs could be used as a potential multimodal bioprobe in bioimaging applications.
Co-reporter:Jiangman Zhen, Dapeng Liu, Xiao Wang, Junqi Li, Fan Wang, Yinghui Wang and Hongjie Zhang
Dalton Transactions 2015 - vol. 44(Issue 5) pp:NaN2430-2430
Publication Date(Web):2014/12/15
DOI:10.1039/C4DT03141E
A fast and facile self-assembly method has been developed to deposit 3–5 nm sized PdxPt1−x (0 ≤ x ≤ 1) nanoparticles (NPs) on Ni(OH)2 nanosheets. The biomolecule L-lysine has been used here as the linker to hybridize PdxPt1−x NPs and Ni(OH)2 nanosheets together. The catalytic properties of the obtained PdxPt1−x/Ni(OH)2 hybrids were evaluated by employing the reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) by NaBH4 as a model reaction. The results reveal that the stability, activity and recyclability of PdxPt1−x NPs have been remarkably enhanced after being supported on Ni(OH)2 nanosheets. Moreover, the influence of the composition of noble metals on the catalytic properties has been studied in depth and Pd0.5Pt0.5/Ni(OH)2 hybrids show the optimal catalytic properties.
Co-reporter:Zhuo Wang, Jing Feng, Shuyan Song, Zhiqiang Sun, Shuang Yao, Xin Ge, Min Pang and Hongjie Zhang
Journal of Materials Chemistry A 2014 - vol. 2(Issue 42) pp:NaN9011-9011
Publication Date(Web):2014/09/08
DOI:10.1039/C4TC01778A
The pure and intense orange upconversion luminescence of Eu3+ was efficiently achieved in NaYF4 and NaLuF4 nanocrystals through the upconversion sensitization of doped Yb3+ and Mn2+ ions dimer for the first time. A shell-coating strategy was performed to further enhance the emission intensity. In this work, a novel upconversion mechanism for energy transfer from the Yb3+–Mn2+ dimer to the Eu3+ ion was proposed by analyzing the upconversion luminescence spectra, lifetimes and pumping photons measurements of the obtained nanocrystals in detail. The applications of the nanocrystals for CT imaging and ratiometric pH sensing in physiological pH range were performed. This study also provides a new upconversion spectral region at around 592 nm for applications in multicolor imaging, multiplexed encoding and detection.
Co-reporter:Xue-Zhi Song, Shu-Yan Song, Min Zhu, Zhao-Min Hao, Xing Meng, Shu-Na Zhao and Hong-Jie Zhang
Dalton Transactions 2013 - vol. 42(Issue 36) pp:NaN13240-13240
Publication Date(Web):2013/06/21
DOI:10.1039/C3DT51241J
Hydrothermal reaction of a tripodal bridging ligand, 5-(4-carboxyphenoxy)isophthalic acid (H3cpia) with cobalt salts modulated by N-donor neutral ligands leads to the formation of six novel coordination networks formulated as {[Co1.5(cpia)(o-bix)](H2O)1.5}n (1), {[Co2(cpia)(μ-OH)(m-bix)]H2O}n (2), {[Co1.5(cpia)(m-bix)]}n (3), {[Co1.5(cpia)(p-bix)0.5(H2O)]H2O}n (4), {[Co2.5(cpia)(Hcpia)(4,4′-bpy)2.5](H2O)3}n (5), and {[Co3(cpia)2(bpp)2]H2O}n (6). Compound 1 exhibits a two-dimensional, (3,8)-connected layered architecture composed of trinuclear cobalt clusters. Compound 2 possesses a three-dimensional dense framework with (3,8)-connected tfz-d topology built from butterfly-shaped tetranuclear Co4(μ3-OH)26+ clusters. Similar to compound 1, trinuclear Co clusters act as secondary building units to construct the final 2D layered structure modulated by m-bix and bpp ligands in compounds 3 and 6. In compound 4, trinuclear Co clusters connected by cpia3− anions give rise to two-dimensional layers, which are further pillared by p-bix ligands to the three-dimensional framework. Compound 5 features a 2D, (3,4,6)-connected molecular network assembled from alternate binuclear and mononuclear Co building blocks. The magnetic investigation indicates that strong antiferromagnetic interactions between cobalt ions are dominant in compounds 2 and 6.
Co-reporter:Fan Wang, Xiao Wang, Dapeng Liu, Jiangman Zhen, Junqi Li and Hongjie Zhang
Dalton Transactions 2015 - vol. 44(Issue 48) pp:NaN21130-21130
Publication Date(Web):2015/11/09
DOI:10.1039/C5DT03360H
In this work, three kinds of ZnCo2O4 morphologies, that is, rod, plate and sphere, have been successfully prepared and further used to support Pt nanoparticles (NPs) via in situ deposition. The as-prepared ZnCo2O4–Pt hybrid nanomaterials were then carefully characterized by SEM, TEM, XRD, XPS, ICP EDX, and N2 adsorption measurement in great detail. Besides, the three catalysts were also evaluated by the model reaction of catalytic CO oxidation. After comparing the difference in the three kinds of morphologies, we have tried to clarify the reason for their different catalytic performances. As a result, the ZnCo2O4–Pt sphere was found to be the most active, attaining 100% CO conversion at a relatively low temperature of 140 °C, because more Pt NPs are prone to distribution on the surface of ZnCo2O4 spheres than the other ones. The following cycling tests confirm the excellent stability of the as-prepared ZnCo2O4–Pt samples.
Co-reporter:Xia Xu, Zhuo Wang, Pengpeng Lei, Xiuling Liu, Yue Su, Lile Dong, Shuang Yao, Liang Zhou, Shuyan Song, Jing Feng and Hongjie Zhang
Dalton Transactions 2015 - vol. 44(Issue 39) pp:NaN17292-17292
Publication Date(Web):2015/09/02
DOI:10.1039/C5DT02751A
Cubic KLu3F10 nanocrystals have been fabricated by doping Mn2+ ions via a liquid–solid solution (LSS) hydrothermal method. With an increase in the Mn2+ level, a phase transformation from orthorhombic KLu2F7 to cubic KLu3F10 associated with evolution of the particle morphologies and sizes is evident. The phase transformation mechanism based on doping with Mn2+ ions was studied via a series of time-controlled experiments and the enhancement of the intensity of upconversion luminescence (UCL) via doping with Mn2+ ions is discussed in detail. In addition, under 980 nm excitation, the UCL properties of Er3+/Tm3+/Ho3+-doped KLu3F10:Yb3+ upconversion nanoparticles (UCNPs) have been investigated and a possible UCL mechanism has been discussed. It has been demonstrated that cubic KLu3F10 is an excellent host for upconversion luminescence.
Co-reporter:Yue Su, Xiuling Liu, Pengpeng Lei, Xia Xu, Lile Dong, Xianmin Guo, Xingxu Yan, Peng Wang, Shuyan Song, Jing Feng and Hongjie Zhang
Dalton Transactions 2016 - vol. 45(Issue 27) pp:NaN11136-11136
Publication Date(Web):2016/06/21
DOI:10.1039/C6DT01005A
Core–shell–shell heterostructures of α-NaLuF4:Yb/Er@NaLuF4:Yb@MF2 (M = Ca, Sr, Ba) have been successfully fabricated via the thermal decomposition method. Upconversion nanoparticles (UCNPs) were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), upconversion luminescence (UCL) spectroscopy, etc. Under 980 nm excitation, the emission intensities of the UCNPs are remarkably enhanced after coating the MF2 (M = Ca, Sr, and Ba) shell. Among these samples, CaF2 coated UCNPs show the strongest overall emission, while BaF2 coated UCNPs exhibit the longest lifetime. These results demonstrate that alkaline earth metal fluorides are ideal materials to improve the UCL properties. Meanwhile, although the lattice mismatch between the ternary NaREF4 core and the binary MF2 (M = Sr and Ba) shell is relatively large, the successfully synthesized NaLuF4:Yb/Er@NaLuF4:Yb@MF2 indicates a new outlook on the fabrication of heterostructural core–shell UCNPs.
Co-reporter:Junqi Li, Shuang Yao, Shuyan Song, Xiao Wang, Yinghui Wang, Xing Ding, Fan Wang and Hongjie Zhang
Dalton Transactions 2016 - vol. 45(Issue 28) pp:NaN11527-11527
Publication Date(Web):2016/06/20
DOI:10.1039/C6DT02044E
Nanomaterials that can restrain or reduce the production of excessive reactive oxygen species such as H2O2 to defend and treat against Alzheimer's disease (AD) have attracted much attention. In this paper, we adopt the strategy of layer-by-layer deposition; namely, first synthesizing available gadolinium-doped ytterbia nanoparticles (Yb2O3:Gd NPs) as cores, and then coating them with silica via the classical Stöber method to prevent leakage and act as a carrier for subsequent ceria deposition and PEGylation, and finally obtain the expected core@shell-structured nanocomposite of PEGylated Yb2O3:Gd@SiO2@CeO2 islands. The nanomaterial has proved not only to be a high-performance dual-modal contrast agent for use in MRI and CT, but also to exhibit excellent catalase mimetic activity, which may help the prognosis, diagnosis and treatment of AD in the future. In addition, scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared (FTIR) spectroscopy characterization have revealed the successful design and synthesis of the cores with remarkable size uniformity, with well-distributed CeO2 islands decorated on the surface of SiO2 shells, and tightly immobilized PEG.
Co-reporter:Pengpeng Lei, Xiuling Liu, Lile Dong, Zhuo Wang, Shuyan Song, Xia Xu, Yue Su, Jing Feng and Hongjie Zhang
Dalton Transactions 2016 - vol. 45(Issue 6) pp:NaN2693-2693
Publication Date(Web):2015/12/23
DOI:10.1039/C5DT04279H
Water-soluble lanthanide (Ln3+) doped Bi2O3 nanospheres have been successfully prepared through a solid-state-chemistry thermal decomposition process. The nanospheres exhibit intense upconversion luminescence (UCL) by doping the Ln3+ (Ln = Yb, Er/Ho/Tm) ions into the Bi2O3 host matrix under 980 nm excitation. The ratio of red/green emission of Bi2O3:Yb3+/Er3+ nanospheres exhibits a significant change as the calcination temperature increases and the value could reach 105.6. Moreover, the UCL of Bi2O3:Yb3+/Tm3+ nanospheres are temperature-sensitive, where the intensity ratios of 799 and 808 nm emissions increase monotonously with temperature. The MTT assay reveals that Bi2O3:Yb3+/Tm3+ nanospheres exhibit good biocompatibility by grafting citric acid molecules on the surface. The application possibility of Bi2O3:Yb3+/Tm3+ nanospheres as bioprobes for optical imaging in vivo is also confirmed by the high-contrast photoluminescence images between the background and the UCL imaging area.
Co-reporter:Shuyan Song, Xiao Wang, Sheling Li, Zhuo Wang, Qi Zhu and Hongjie Zhang
Chemical Science (2010-Present) 2015 - vol. 6(Issue 11) pp:NaN6424-6424
Publication Date(Web):2015/07/23
DOI:10.1039/C5SC01686J
Recent studies have further demonstrated that the conjugation of noble metal helical nanostructures could alter their optical and catalytic activities. However, the intrinsic isotropic crystal growth of Pt makes the synthesis of high-quality Pt NCs with unique porous or branched nanostructures difficult. In this work, a new, powerful capping agent, N,N-dimethyloctadecylammonium bromide acetate sodium, was synthesized and used to coordinate Pt ions, slowing down the reaction rate. As a result, in aqueous solution, Pt nanohelices with highly ordered horizontal pore channels were successfully fabricated. Importantly, the Pt nanohelices were composed of several sub-2 nm Pt nanowires coiled together around a central point. The as-obtained samples exhibited enhanced photothermal properties compared with the classic Pt nanoparticles.
Co-reporter:Yinghui Wang, Xing Ding, Fan Wang, Junqi Li, Shuyan Song and Hongjie Zhang
Chemical Science (2010-Present) 2016 - vol. 7(Issue 7) pp:NaN4290-4290
Publication Date(Web):2016/03/09
DOI:10.1039/C5SC04668H
To tackle the issues of inferior cycling stability and low conductivity for MnO as an anode material for lithium ion batteries (LIBs) and as a catalyst for oxygen reduction reaction (ORR), a facile and effective strategy is explored to confine N-doped carbon-coated MnO nanoparticles in a conductive graphene matrix. The synthesis of the GMNCs involves the two-step coating of Mn3O4 nanocrystals with polydopamine and graphene, followed by heat treatment to form the GNS@MnO@N-doped carbon composites (GMNCs). When evaluated as anode materials for LIBs, the as-prepared GMNCs exhibit an improved cycling stability (754.3 mA h g−1 after 350 cycles at 0.1 A g−1) compared to carbon-coated MnO and pure Mn3O4 due to the double carbon coating design. When evaluated as catalysts for ORR, the as-prepared GMNCs exhibit higher electrocatalytic activity than that of pure Mn3O4 and MnO catalysts, and superior stability to a commercial Pt/C catalyst due to the synergetic effect between the MnO and N-doped double carbon coating. The optimum design of the unique nanostructures with the synergetic effect provides a new route to design advanced materials as electrode/catalysts for energy conversion and storage.
Co-reporter:Xing Meng, Xue-Zhi Song, Shu-Yan Song, Guo-Cheng Yang, Min Zhu, Zhao-Min Hao, Shu-Na Zhao and Hong-Jie Zhang
Chemical Communications 2013 - vol. 49(Issue 76) pp:NaN8485-8485
Publication Date(Web):2013/07/16
DOI:10.1039/C3CC44106G
3D pillar-layer framework 1 with [24-MC-6] heterometallic crown clusters exhibits proton conductivity and selective sensing of acetone as well as Cu2+ ions.
Co-reporter:Zhiyong Guo, Xuezhi Song, Huaping Lei, Hailong Wang, Shengqun Su, Hui Xu, Guodong Qian, Hongjie Zhang and Banglin Chen
Chemical Communications 2015 - vol. 51(Issue 2) pp:NaN379-379
Publication Date(Web):2014/11/10
DOI:10.1039/C4CC06729K
A ketone functionalized luminescent terbium metal–organic framework has been realized for the highly selective and sensitive sensing of aniline.
Co-reporter:Xia Xu, Xuesong Zhai, Kaimin Du, Pengpeng Lei, Lile Dong, Ruiping Deng, Jing Feng and Hongjie Zhang
Journal of Materials Chemistry A 2017 - vol. 5(Issue 25) pp:NaN6318-6318
Publication Date(Web):2017/05/22
DOI:10.1039/C7TC01586K
Impurity doping has a significant influence on the nucleation and growth of nanocrystals. The influence of the ionic radius of the dopant and grain size on the crystallographic phase of KLu2F7:Yb3+/Er3+ nanocrystals has not been systematically investigated. Herein, we demonstrate an M ion (M = Mn2+, Gd3+, Nd3+) doping approach to dynamically fine-tune the grain size of KLu2F7:Yb3+/Er3+ nanocrystals, and study the influence of the ionic radius of the doping M ions and particle size reduction on the crystallographic phase. Through a comprehensive investigation of the impurity doping induced phase transition phenomenon and the growth mechanism of KLu2F7:Yb3+/Er3+ nanocrystals, we speculated that the impurity doping induced phase transition mechanism of KLu2F7:Yb3+/Er3+ mainly depends on the grain size of nanocrystals ignoring the ionic radius of the dopant. With the decrease of the grain size, high surface tension triggers phase transformation from anisotropic (orthorhombic KLu2F7:Yb3+/Er3+) to isotropic (cubic KLu3F10:Yb3+/Er3+). What is more, we have systematically investigated the visible (VIS)-upconversion and near infrared (NIR)-downshifting emission of various-sized KLu2F7:Yb3+/Er3+ UCNPs and Mn2+, Gd3+ or Nd3+ ion doped KLu2F7:Yb3+/Er3+ UCNPs. The findings provide keen insights into understanding the effect of size reduction on the phase transition mechanism and the photoluminescence properties of KLu2F7:Yb3+/Er3+ UCNPs, while offering the possibility for good academic studies and application prospects.