Co-reporter:F. Li;L. Zhang;X. Chen;Y. L. Liu;S. G. Xu;S. K. Cao
Physical Chemistry Chemical Physics 2017 vol. 19(Issue 32) pp:21862-21868
Publication Date(Web):2017/08/16
DOI:10.1039/C7CP03995F
A N and Fe codoped monoclinic BiVO4 (N–Fe-BVO) photocatalyst was prepared via a conventional sol–gel method and was evaluated for the photocatalytic reduction of CO2 with H2O under visible-light irradiation (>400 nm). As revealed by the structural and photoelectric characterization, the doped N and Fe species can enter the lattice of BiVO4 and induce the codopant levels in the forbidden region of BiVO4, which helps in increasing visible-light absorption, suppressing charge recombination and promoting charge migration. Compared to pure or single-doped BiVO4, the N–Fe-BVO photocatalyst exhibited substantially improved visible-light photocatalytic activity for CO2 reduction, with the highest hydrocarbon generation rate of 27 μmol h−1 gcat−1 and the corresponding quantum efficiency of 1.86% being obtained. The enhanced photocatalytic activity of N–Fe-BVO can be attributed to the synergistic effect of the simultaneous presence of the Fe and N dopants, and the possible photocatalytic mechanism was also proposed based on the characterization results.
Co-reporter:Shengang Xu, Chong Fang, Yanzhao Wu, Wenbo Wu, Qing Guo, Jin Zeng, Xuezhao Wang, Yingliang Liu, Shaokui Cao
Dyes and Pigments 2017 Volume 142(Volume 142) pp:
Publication Date(Web):1 July 2017
DOI:10.1016/j.dyepig.2017.03.001
•Seven CRA-based photorefractive (PR) hyper-structured molecular glasses (HSMGs) were synthesized by esterification.•The degrees of introduction of bulky NLO chromophores to the CRA core were higher than 70%.•The Γ values of HSMGs composites are about two times of the corresponding small molecular functional compounds composite.•The Γ value of CRA-CSN/ECz/PCBM (69:30:1, wt.%) composite was 78.2 cm−1 at the external electric field of 12.5 V mm−1.Seven C-methylcalix[4]resorcinarene (CRA)-based photorefractive (PR) hyper-structured molecular glasses (HSMGs) containing carbazole-based methine nonlinear optical (NLO) chromophores were designed and synthesized via esterification between carboxyl-containing asymmetric CRA core molecule and hydroxyl-containing functional compounds. When the feed ratio of hydroxyl-containing NLO functional compounds to carboxyl groups of CRA-COOH was kept at 1.5/1 by mole, the degree of introduction of NLO chromophore to the CRA core was above 70%. All the HSMGs show low glass transition temperatures (Tg), and good solubility in common low boiling point solvents such as THF, CHCl3, etc. Powder XRD and UV–vis absorption in films of HSMGs indicate that the aggregation, packing and crystallization of the NLO chromophores in these HSMGs had been effectively reduced. Doping with N-ethyl-carbazole (ECz) as a plasticizer and [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) as a photosensitizer, all the HSMGs composites showed good PR effects. All the coupling gain coefficients (Γ) of HSMGs-based composites are about twice to the corresponding small molecular NLO chromophores-based composites, thanks to the decreased NLO chromophores antiparallel packing caused by the asymmetric CRA core. Among them, CRA-CSN/ECz/PCBM (69:30:1, wt%) composite exhibited the best performance with the Γ value of 78.2 cm−1 at the external electric field of 12.5 V μm−1, which is one of the best performance in molecular glasses under the same test conditions. Coupled with their convenient synthesis, this work will provide a new simple design strategy for organic PR materials.C-methylcalix[4]resorcinarene(CRA)-based photorefractive (PR) hyper-structured molecular glasses (HSMGs) containing carbazole-based methine nonlinear optical (NLO) chromophores were designed and synthesized by the esterification between carboxyl-containing asymmetric CRA core molecule and hydroxyl-containing NLO functional compounds. All the two beam coupling gain coefficients of HSMGs composites are about two times of the corresponding NLO functional compounds composite due to the decrease of NLO chromophores antiparallel packing caused by the asymmetric CRA core.Download high-res image (187KB)Download full-size image
Co-reporter:Han Li, Chao Liang, Yingliang LiuYiqiang Zhang, Jincheng Tong, Weiwei Zuo, Shengang Xu, Guosheng Shao, Shaokui Cao
ACS Applied Materials & Interfaces 2017 Volume 9(Issue 7) pp:
Publication Date(Web):January 26, 2017
DOI:10.1021/acsami.6b15434
Grain boundaries act as rapid pathways for nonradiative carrier recombination, anion migration, and water corrosion, leading to low efficiency and poor stability of organometal halide perovskite solar cells (PSCs). In this work, the strategy suppressing the crystal grain boundaries is applied to improve the photovoltaic performance, especially moisture-resistant stability, with polyvinylammonium carbochain backbone covalently connecting the perovskite crystal grains. This cationic polyelectrolyte additive serves as nucleation sites and template for crystal growth of MAPbI3 and afterward the immobilized adjacent crystal grains grow into the continuous compact, pinhole-free perovskite layer. As a result, the unsealed PSC devices, which are fabricated under low-temperature fabrication protocol with a proper content of polymer additive PVAm·HI, currently exhibit the maximum efficiency of 16.3%. Remarkably, these unsealed devices follow an “outside-in” corrosion mechanism and respectively retain 92% and 80% of the initial PCE value after being exposed under ambient environment for 50 days and 100 days, indicating the superiority of carbochain polymer additives in solving the long-term stability problem of PSCs.Keywords: covalently connecting; long-term stability; perovskite solar cell; polyvinylammonium; suppressed boundary;
Co-reporter:Xuezhao Wang, Yuanhua Xiao, Dangcheng Su, Liming Zhou, Shide Wu, Lifeng Han, Shaoming Fang, Shaokui Cao
Electrochimica Acta 2016 Volume 194() pp:377-384
Publication Date(Web):10 March 2016
DOI:10.1016/j.electacta.2016.02.047
A new core-shell nanostructure of CoO@MnO2nanowire@nanosheetarrays(NNSs) was designed and directly grown on a 3D nickel foam by a simple two step solution method combined with a post annealing treatment in Ar gas. The MnO2 nanosheets can grow directly on the CoO precuor nanowires without any pretreatment, and its thickness on the CoO nanowire arrays (NAs) can also be tailored by easily adjusting the second step hydrothermal time. When acting as a electrochemical supercapacitor, the CoO@MnO2 NNAs delivers a highly enhanced specific capacitance of 3.03 F cm−2 (about 1515 F g−1) with a wide potential window of 0.8 V at 2.0 mA cm−2, which is superior to most reported Co3O4 based core-shell NNAs supercapacitive electrodes. An asymmetric supercapacitor devices based on these CoO@MnO2 NNAs and aqueous electrolyte showed with a high-energy density of 0.37 mWh cm−2 at a power density of 1.7 mW cm−2, a high power density of 34.4 mW cm−2 at 0.20 mWh cm−2 and a long-term cycling ability, implying its great potential application in high-performance electrochemical supercapacitor.
Co-reporter:Yingliang Liu, Zhenru Zhang, Xuemei Chen, Shengang Xu, Shaokui Cao
Dyes and Pigments 2016 Volume 128() pp:179-189
Publication Date(Web):May 2016
DOI:10.1016/j.dyepig.2016.01.026
•Soluble dithiolene nickel complexes are synthesized as NIR absorbing dyes.•Dithiolene ligands in carbazole-containing nickel complex take radical monoanion.•Substituent electron-donating ability changes chemical state of molecular core.•The resulting complexes take on a glassy state at low temperature.•Dithiolene nickel complexes could be applied to NIR laser protection at 1064 nm.Soluble dithiolene nickel complexes are designed and synthesized as near-infrared (NIR) absorbing dyes through the introduction of strong electron-donating groups at the molecular periphery. The resulting complexes are characterized by 1H/13C NMR, IR, ESI-MS, UV–vis–NIR, TG, DSC, XPS and elemental analysis. The identification results are in accord with the chemical structure of designed dithiolene nickel complexes. The XPS results suggested that the dithiolene ligands in carbazole-containing nickel complex take a radical monoanion, which depends on the substituent electron-donating ability to a large extent. The TG and DSC measurements indicated that the resulting complexes have an excellent thermal stability and take on a glassy state at low temperature. The laser transmittance measurement suggested that the optical filters fabricated through static solution-casting approach with dithiolene nickel complexes as NIR absorbing dyes could be well applied to the NIR laser protection at 1064 nm.
Co-reporter:Xuezhao Wang, Yuanhua Xiao, Dangcheng Su, Shengang Xu, Liming Zhou, Shide Wu, Lifeng Han, Shaoming Fang, Shaokui Cao
International Journal of Hydrogen Energy 2016 Volume 41(Issue 31) pp:13540-13548
Publication Date(Web):17 August 2016
DOI:10.1016/j.ijhydene.2016.06.133
•CoO@MnO2 core-shell nanoarray was prepared by a novel solvothermal reaction without pre-carbonization treatment.•Density of MnO2 nanosheets on the CoO nanosheets can be tailored.•The CoO@MnO2 delivers an ultra-high areal specific capacitance of 2.40 F cm−2.•The asymmetric supercapacitor achieves a high-energy density of 1.4 mWh cm−3.•Excellent long-term stability: 90.0% capacitance retention after 10 000 cycles.Hierarchical hybrid electrodes CoO@MnO2 nanosheet@nanosheet arrays (NNAs) for high-performance supercapacitors are designed and grown on a 3D nickel foam by a simple two step solution method combined with a post annealing treatment in Ar gas. The MnO2 nanosheets can grow directly on the CoO precursor nanosheet arrays without any pretreatment, and its thickness on the CoO NAs can also be tailored by adjusting the hydrothermal time. The NNAs with the elegant synergy between CoO and MnO2 lead to a highly enhanced areal capacitance (2.40 F cm−2 at 2.0 mA cm−2, with a wide potential window of 0.8 V). We further fabricated asymmetric supercapacitor device based on the CoO@MnO2 NNAs and active carbon, which achieved a high-energy density of 1.4 mWh cm−3 at a power density of 9.6 mW cm−3, a high power density of 192.3 mW cm−3 at 0.7 mWh cm−3 and good cyclic stability.
Co-reporter:Shuya Gao, Li Zhang, Yadong Qiao, Pei Dong, Jun Shi and Shaokui Cao
RSC Advances 2016 vol. 6(Issue 64) pp:58854-58861
Publication Date(Web):13 Jun 2016
DOI:10.1039/C6RA06263F
The construction of a 3D graphene-based hybrid electrode with an optimized porous structure remains an attractive topic. Herein, we used the highly conductive graphene hydrogel (GH) with a well-defined 3D macroporous structure as a support to electrodeposite polyaniline (PANI), aimed to improve the energy density of GH-based capacitor electrode without deteriorating its high power capability. The as-prepared GH/PANI heterostructure with thin PANI layer conformally coated on the GH framework totally retains the native hydrogel pore structure and its high surface area, which facilitates the effective electron and ion transport within the electrode and thus endows GH/PANI composite electrode with excellent electrochemical properties such as a specific capacitance of 710 F g−1 at 2 A g−1 and 73% capacitance retention upon a current increase to 100 A g−1. Moreover, the assembled symmetric supercapacitor device based on GH/PANI heterostructure electrode delivers a maximum energy density and power density of 24 W h kg−1 and 30 kW kg−1, respectively, and also exhibits a good cycling stability with 86% capacitance retention after 1000 cycles. These findings demonstrate the importance and great potential of GH-based heterostructure in the development of high-performance energy-storage systems.
Co-reporter:Shuhan Xu;Jun Shi;Liu Yang;Qiong Wu
Journal of Applied Polymer Science 2016 Volume 133( Issue 7) pp:
Publication Date(Web):
DOI:10.1002/app.43008
ABSTRACT
In this work, smart hollow microcapsules made of thermal-/pH-dual sensitive aliphatic poly(urethane-amine) (PUA), sodium poly(styrenesulfonate) (PSS), and Au nanoparticles (AuNPs) for interdependent multi-responsive drug delivery have been constructed by layer-by-layer (LbL) technique. The electrostatic interactions among PUA, PSS, and AuNPs contribute to the successful self-assembly of hollow multilayer microcapsules. Thanks to the shrinkage of PUA above its lower critical solution temperature (LCST) and the interaction variation between PUA and PSS at different pH conditions, hollow microcapsules exhibit distinct pH- and thermal-sensitive properties. Moreover, AuNPs aggregates can effectively convert light to heat upon irradiation with near-infrared (NIR) laser and endow the hollow microcapsules with distinct NIR-responsiveness. More importantly, the NIR-responsive study also demonstrates that the microcapsule morphology and the corresponding NIR-responsive drug release are strongly dependent on the pH value and temperature of the media. The results indicate that the prepared hollow PUA/PSS/Au microcapsules have the great potential to be used as a novel smart drug carrier for the remotely controllable drug delivery. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 43008.
Co-reporter:Fei Li, Li Zhang, Jincheng Tong, Yingliang Liu, Shengang Xu, Yan Cao, Shaokui Cao
Nano Energy 2016 Volume 27() pp:320-329
Publication Date(Web):September 2016
DOI:10.1016/j.nanoen.2016.06.056
•Monolithic two-side Cu2O/graphene/TNA heterostructure photocatalyst was prepared.•CO2 photoreduction was achieved in a visible-light-driven dual-chamber reactor.•Methanol yield of 45 μmol cm−2 h−1 and quantum efficiency of 5.71% was attained.•The reaction mechanism and stability of the ternary heterostructure is explored.Efficient photocatalytic CO2 conversion to methanol under visible light irradiation (λ>400 nm) was achieved in a light-driven dual-chamber reactor using the monolithic two-side Cu2O/graphene/TiO2 nanotube array (TNA) heterostructure as separated oxidation and reduction catalyst, that was prepared with anodic TNA as the substrate following by sequential electrochemical deposition of graphene and Cu2O. The combined heterojunction in the ternary composite helps to improve the photocatalytic performance by increasing light absorption, preventing electron–hole recombination and facilitating electron transfer across the heterojunction interfaces, as revealed by photoelectrochemical measurements. Methanol generation rate of 45 μmol cm−2 h−1 was achieved, which is much higher than those obtained for existing TNA-based photocatalysts reported. Moreover, the quantum efficiency of 5.71% at 420 nm has been attained. The improved photocatalytic activity together with the proposed reaction mechanism demonstrated the advantage of Cu2O/graphene/TNA heterostructure and effectiveness of the reaction system, which can efficiently suppress charge recombination, improve interfacial charge transfer and inhibit the backward reaction by separating the photocatalytic reaction sites.Achieving efficient photocatalytic CO2 conversion to methanol in a visible-light-driven dual-chamber reactor with monolithic Cu2O/graphene/TNA heterostructure photocatalyst.
Co-reporter:Jing Wei, Jun Shi, Qiong Wu, Liu Yang and Shaokui Cao
Journal of Materials Chemistry A 2015 vol. 3(Issue 41) pp:8162-8169
Publication Date(Web):01 Sep 2015
DOI:10.1039/C5TB01268F
Hybrid hydroxyapatite (HAP) microparticles with a hollow HAP core and a chitosan/hyaluronic acid (CHI/HA) multilayer shell were fabricated via the hydrothermal method and the layer-by-layer (LbL) self-assembly technique. Depending on the hydrothermal reaction time, the thickness of the HAP shell could be controlled and the size of the hybrid hollow microparticles varied between 850 nm and 2 μm. The size and HAP shell thickness significantly affect the drug release property of the resulting hybrid microparticles. The DOX release results demonstrated that CHI/HA multilayers could potentially assuage the initial burst release of drug from the porous HAP matrix because the polymer multilayer shell acted as a barrier to control the exchange of the drug. In addition, the drug release of hollow hybrid HAP microparticles was pH-dependent because of the different electrostatic interaction in the CHI/HA multilayers at different pH values and the dissolution of the HAP hollow core under acidic conditions. The present paper provides a facile and green route for the fabrication of hierarchical hybrid drug carriers with controllable size, wall thickness and drug release properties by combining natural polyelectrolytes and hollow HAP microparticles, which is highly attractive for controllable drug delivery.
Co-reporter:Jincheng Tong, Li Zhang, Fei Li, Mingming Li and Shaokui Cao
Physical Chemistry Chemical Physics 2015 vol. 17(Issue 36) pp:23532-23537
Publication Date(Web):14 Aug 2015
DOI:10.1039/C5CP04057D
Graphitic carbon nitride (g-C3N4) nanosheets with large aspect ratios were fabricated from bulk g-C3N4 through an efficient top-down approach of moderate disintegration–exfoliation using diluted H2SO4 as an “efficient knife”. By prior disintegration in a diluted H2SO4 solution, the exfoliation of bulk g-C3N4 was effectively accelerated. The as-prepared g-C3N4 nanosheets possess a two-dimensional (2D) thin-layer structure with seven-atom thickness, a large lateral size of about 1 μm, and a high specific surface area of 80 m2 g−1. Compared with the bulk precursor, the g-C3N4 nanosheets showed much higher efficiency of photogenerated charge transfer and separation, and consequently exhibited enhanced photocatalytic activity toward hydrogen evolution and pollutant decomposition under both full-sunlight and visible-light irradiation.
Co-reporter:Jincheng Tong, Li Zhang, Fei Li, Ke Wang, Lifen Han and Shaokui Cao
RSC Advances 2015 vol. 5(Issue 107) pp:88149-88153
Publication Date(Web):12 Oct 2015
DOI:10.1039/C5RA16988G
Rapid and high-yield production of graphitic carbon nitride (g-C3N4) nanosheets was realized by simply adding water into a H2SO4 suspension of bulk g-C3N4, and the as-prepared nanosheets exhibit enhanced photocatalytic H2 evolution. Notably, the degree of exfoliation can be controlled by the amount of water to facilitate diverse applications of nano-sized g-C3N4.
Co-reporter:Qiong Wu, Jun Shi, Jing Wei, Liu Yang and Shaokui Cao
RSC Advances 2015 vol. 5(Issue 86) pp:70101-70108
Publication Date(Web):12 Aug 2015
DOI:10.1039/C5RA13630J
In this work, aliphatic poly(urethane-amine) (PUA) grafted mesoporous hollow hydroxyapatite (H-HAP) microparticles were prepared via in situ polymerization in supercritical CO2. Thermal-responsive PUA acted as the on–off gates inside the mesoporous H-HAP due to the stretch and shrinkage of the PUA polymer chains at different temperatures. The PUA-grafted hollow HAP (PUA-g-H-HAP) microparticles displayed high specific surface area (95 m2 g−1) and drug loading efficiency (60%). The in vitro drug release studies indicated that PUA-g-H-HAP microparticles exhibited distinguishable pH- and thermal-dependent drug release properties, and PUA on–off switches enabled the DOX release in a reversible way by simply adjusting the environmental temperature. Moreover, compared to the hollow HAP microparticles having a higher amount of released DOX over the initial 2 h (about 24.4% of total released drug over 24 h) at 37 °C and pH 7.4, PUA-g-H-HAP microparticles displayed a sustained release property with the value of only 10.7% deriving from the blockage of the stretched PUA chains inside the mesoporous H-HAP.
Co-reporter:Yuxia Jin;Weiwei Zuo;Hongyan Gao;Linfeng Fu;Yingliang Liu;Wenbo Wu;Shengang Xu
Journal of Applied Polymer Science 2015 Volume 132( Issue 46) pp:
Publication Date(Web):
DOI:10.1002/app.42746
ABSTRACT
A novel carbazole–triphenylamine copolymer-bearing pendant bipyridine PM1TPA and corresponding europium (III) complexed polymer PM1TPA–Eu–x, in which the values of x are 0.1, 0.5, and 1.0 representing the molar ratio of bipyridine ligands complexed with Eu(III), were designed and synthesized. Their chemical structures were confirmed by 1H NMR, FT-IR, and elemental analysis. Both PM1TPA and PM1TPA–Eu shows good solubility in common organic solvents such as tetrahydrofuran (THF) and CHCl3. The 5% weight loss temperature (Td5%) of PM1TPA and PM1TPA–Eu–1.0 are 363oC and 306oC, respectively. The photoluminescence (PL) spectra of PM1TPA–Eu in solution consists of two emission bands, one in the 400–570 nm region and another at 612 nm, corresponding to the emission of polymer main chain and europium complexes, respectively. When the concentration of PM1TPA–Eu–1.0 in THF solution increases, the PL intensity in the 400–570 nm regions became more and more weaker. And only the characteristic emission of europium complex was observed in the solid film, which indicates that the excited energy absorbed by the polymer backbone was efficiently transferred to the europium complexes. Furthermore, nearly monochromatic red electroluminescence from europium complex was observed from the polymeric light-emitting diode using PM1TPA–Eu–1.0 as the emissive layer under 25 V forward bias. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015, 132, 42746.
Co-reporter:Yingliang Liu, Shengping Wang, Shengang Xu, Shaokui Cao
Materials Research Bulletin 2015 65() pp: 27-35
Publication Date(Web):
DOI:10.1016/j.materresbull.2015.01.031
Co-reporter:Shaoling Xia, Yingliang Liu, Fuyun Pei, Linqi Zhang, Qiuju Gao, Wenjun Zou, Jin Peng, Shaokui Cao
Polymer 2015 Volume 64() pp:62-68
Publication Date(Web):1 May 2015
DOI:10.1016/j.polymer.2015.03.036
•GO-hybrided PU/EP IPNs are prepared through an in-situ polymerization.•The friction coefficient is decreased about 30.2% due to GO-hybridization.•The specific wear rate is decreased about two orders of magnitude.•The same friction coefficient in steady stage is obtained independent of GO content.•The identical steady friction coefficients are derived from the same friction bodies.Graphene-oxide-hybrided polyurethane/epoxy interpenetrating polymer networks (PU/EP IPNs) are prepared through an in-situ polymerization. The results showed that the mechanical performance of graphene-oxide-hybrided PU/EP IPNs is improved due to the formation of chemical bonds between graphene oxide nanosheet and polyurethane/epoxy segments, affording the loading transfer from polymer matrix to graphene oxide nanosheet. The average friction coefficient in the steady stage is decreased about 30.2% from neat PU/EP IPN to graphene-oxide-hybrided PU/EP IPNs. Especially, the specific wear rate is decreased about two orders of magnitude from neat PU/EP IPN to graphene-oxide-hybrided PU/EP IPNs. Interestingly, graphene-oxide-hybrided PU/EP IPNs have the same friction coefficient in the steady stage, independent of graphene oxide content. The identical steady friction coefficients are derived from the same friction bodies in three-body friction model, such as graphene-oxide-strengthened PU/EP IPN surface, metallic counterpart and graphene-oxide-wrapping polymer particles as wear debris in the transfer film.
Co-reporter:Yingliang Liu, Yue Zhao, Shengang Xu, Shaokui Cao
Polymer 2015 Volume 77() pp:42-47
Publication Date(Web):23 October 2015
DOI:10.1016/j.polymer.2015.09.014
•Ionic liquid [BMIm]Cl is doped into PEDOT:PSS to adjust the performance of OLEDs.•UPS results indicated the decrease of ionization potential of IL-doped PEDOT:PSS.•SEM observation showed the phase transition of IL-doped PEDOT:PSS.•The optimal luminous efficiency is enhanced about 5.0 times due to IL-doping.Ionic liquid (IL) 1-butyl-3-methylimidazolium chloride ([BMIm]Cl) is doped into PEDOT:PSS hole-injecting layer to adjust the electroluminescent performance of OLEDs. The secondarily IL-doped PEDOT:PSS films are characterized in detail by SEM, XPS and UPS. The UPS results indicated the decrease of ionization potential of PEDOT:PSS due to the secondary IL-doping. The SEM observation showed the phase transition of IL-doped PEDOT:PSS films from the crazing texture to smoothing surface and serious phase separation. As a result, the IL-doped PEDOT:PSS allows the optimal luminous efficiency to reach a maximum value of 4.27 cd/A, which is about 5.0 times as 0.85 cd/A in the IL-undoped PEDOT:PSS hole-injecting layer.
Co-reporter:Yuxia Jin, Yingliang Liu, Wenbo Wu, Qiong Wu, Hongyan Gao, Chenxu Wang, Shengang Xu, Shaokui Cao
Reactive and Functional Polymers 2015 90() pp: 7-14
Publication Date(Web):
DOI:10.1016/j.reactfunctpolym.2015.02.008
Co-reporter:Shuhan Xu, Jun Shi, Desheng Feng, Liu Yang and Shaokui Cao
Journal of Materials Chemistry A 2014 vol. 2(Issue 38) pp:6500-6507
Publication Date(Web):30 Jul 2014
DOI:10.1039/C4TB01066C
In this study, hollow hierarchical hydroxyapatite (HAP)/Au/polyelectrolyte hybrid microparticles with a hollow HAP core and polymer multilayer/Au nanoparticle (AuNPs) shell for multi-responsive drug delivery have been prepared via a layer-by-layer (LbL) technique. Thermal-/pH-dual responsive aliphatic poly(urethane-amine) (PUA) was employed as the smart component. The aggregated AuNPs inside hybrid microparticles could potentially obstruct the diffusion of doxorubicin hydrochloride (DOX) from the hollow microparticles and assuage the initial burst release of DOX. Upon irradiation with near-infrared (NIR) laser, AuNP aggregates can effectively convert light to heat and result in the rapid release of DOX due to the partial collapse of the polyelectrolyte multilayers (PUA/sodium poly(styrenesulfonate) (PSS)). In addition, due to the dissolution of HAP in the acidic media and the shrinkage of aliphatic PUA above its lower critical solution temperature (LCST), the drug release of hollow hybrid carriers exhibits distinguished pH- and thermal-dependent properties. The results indicate that the hollow HAP/Au/PUA/PSS hybrid microparticles show great potential as novel smart drug carriers for controllable drug delivery.
Co-reporter:Fuyun Pei, Shengang Xu, Wei Zuo, Zhenru Zhang, Yingliang Liu, Shaokui Cao
International Journal of Hydrogen Energy 2014 Volume 39(Issue 13) pp:6845-6852
Publication Date(Web):24 April 2014
DOI:10.1016/j.ijhydene.2014.02.173
•Nanocomposite is synthesized through a in-situ solvothermal nitrogen-doping strategy.•Wrinkled N-graphene nanosheet is stretched by anchoring N-TiO2 nanoparticles.•N-graphene is N-doped again while TiO2 is nitrogen-doped.•Re-doped N-graphene is more ordered than separate N-graphene.•The photocatalytic efficiency of hydrogen generation is improved.Nanocomposite NTNG composed of nitrogen-doped titanium dioxide (N-TiO2) and nitrogen-doped graphene (N-graphene) is synthesized to increase the photocatalytic efficiency for hydrogen production through a convenient in-situ solvothermal nitrogen-doping strategy. TEM and AFM images suggested that NTNG nanosheet consists of approximately 1–5 layers by folding its own sheet and that the wrinkled multilayer textures are stretched to a large extent due to the uniformly anchored N-TiO2 nanoparticles on N-graphene surface effectively avoiding the aggregation. XPS results indicated that the in-situ solvothermal nitrogen-doping not only allows the nitrogen-doping of TiO2 but also further changes the nitrogen-doping state of N-graphene including the nitrogen content and the ratio of dopant types. Raman spectroscopy told us that N-graphene in NTNG is more ordered than separate N-graphene due to fewer defects from the improved sp2-hybridized nitrogen. As a result, the photocatalytic efficiency of NTNG under ultraviolet irradiation is improved about 13.1 times compared to commercial P25.
Co-reporter:Shaoling Xia;Yingliang Liu;Linqi Zhang;Dongmei Wang;Wenjun Zou;Jin Peng
Journal of Applied Polymer Science 2014 Volume 131( Issue 10) pp:
Publication Date(Web):
DOI:10.1002/app.40244
ABSTRACT
The excellent synergistic effect of physical/mechanical properties of polyurethane/epoxy (PU/EP) interpenetrating polymer network (IPN) and the validity of nanofilling have one potential to improve the wear resistance of polymeric materials. With the aim of practical application, PU/EP IPN nanocomposites are prepared with nanodiamond (ND) as a reinforcing additive. Results showed the uniform thermal stability and the excellent compatibility between PU and EP in ND-hybridized PU/EP IPN. Simultaneously, ND particles work as crosslinked points improving the physical/mechanical properties of ND-hybridized PU/EP IPN, especially the wear resistance. The measurement of tribological property and the scanning electron microscope indicated that the wear resistance is able to be improved a lot by the formation of IPN and by the addition of ND. Consequently, the tribological mechanism of PU/EP IPN nanocomposites comes into being. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40244.
Co-reporter:Jin Shi;Jun Shi;Desheng Feng;Pei Yue
Polymer Bulletin 2014 Volume 71( Issue 7) pp:1857-1873
Publication Date(Web):2014 July
DOI:10.1007/s00289-014-1160-z
CaCO3/aliphatic poly(urethane-amine) (PUA)/sodium polystyrene sulfonate (PSS) hybrid composites with dual-responsive controlled drug delivery property had been prepared via electrostatic interaction. Aliphatic PUA and PSS were employed as smart polyelectrolytes. PSS was also served as crystal growth additive to control the morphology of CaCO3 microparticles. The electrostatic interaction between PSS and aliphatic PUA under weak-acid condition improved the bonding force between PSS-doped CaCO3 microparticles and polyelectrolytes. pH-/thermo-responsive drug delivery property and the high drug loading capacity (around 90 %) could be achieved from the prepared hybrid composites. More importantly, the relative content of CaCO3 microparticles and polyelectrolytes had a significant effect on the morphology and controllable release properties of the hybrid composites. The smart drug release mechanism of the hybrid composites was also analyzed by fitting the cumulative release data to Retger–Peppas equation.
Co-reporter:Lina Zou, Yinfeng Li, Shaokui Cao, Baoxian Ye
Talanta 2014 Volume 129() pp:346-351
Publication Date(Web):1 November 2014
DOI:10.1016/j.talanta.2014.05.057
•DNA/PAn film was modified on the GCE using Langmuir–Blodgett technique.•The sensor was applied to voltammetric detection of xanthine.•Electrochemical properties of xanthine at the sensor were investigated.•The sensor has good sensitivity and selectivity towards xanthine.•The sensor can determine xanthine in human serum samples.DNA–polyaniline (PAn) complex Langmuir–Blodgett film modified glassy carbon electrode (GCE) was used as a new voltammetric sensor (DNA/PAn-LB/GCE) for xanthine (XA) detection. The characteristic of DNA/PAn-LB film was studied by electrochemical impedance spectroscopy and scanning electron microscope. Electrochemical behaviors of XA at the sensor were studied in pH 7.0 phosphate buffer solutions by cyclic voltammetry and differential pulse anodic voltammetry. The results showed that this new modified electrode exhibited an excellent immunity from uric acid and hypoxanthine interference and a new sensitive and selective electroanalytical method for XA was proposed with wider linear range. Under the optimum conditions, the calibration curve for XA was obtained over the range of 7.0×10−8–1.0×10−5 mol L−1, with the detection limit of 3.0×10−8 mol L−1. The practicability of this method was demonstrated by determining the concentration of XA in human serum samples.A new voltammetric sensor DNA/PAn-LB/GCE was designed and successfully used in the determination of xanthine (XA) being free of interference from excess uric acid (UA) and hypoxanthine (HXA).
Co-reporter:Yingliang Liu, Fuyun Pei, Ruijuan Lu, Shengang Xu, Shaokui Cao
Materials Research Bulletin 2014 60() pp: 188-194
Publication Date(Web):
DOI:10.1016/j.materresbull.2014.07.047
Co-reporter:Jun Shi, Jin Shi, Chao Du, Qun Chen, Shaokui Cao
Journal of Membrane Science 2013 Volume 433() pp:39-48
Publication Date(Web):15 April 2013
DOI:10.1016/j.memsci.2013.01.021
Alginate/CaCO3 hybrid membranes with pH- and thermal-responsive drug release properties were prepared under compressed CO2 using polyacrylic acid (PAA) as a crystal growth additive. Aliphatic poly(urethane-amine) (PUA) was employed as the thermal-responsive composition in the hybrid membranes. The hybrid membranes were characterized by scanning electron microscopy, energy dispersive X-ray spectrometer, X-ray diffraction and thermogravimetric analyzer. The interaction between PAA and aliphatic PUA contributed the formation of compact CaCO3 microparticles and the high drug loading efficiency of the hybrid membranes. By adjusting the pressure and reaction time of the biomineralization process, sustained drug release property could be achieved from the hybrid membranes. The results indicated that the compact CaCO3 microparticles could hinder the permeability of the encapsulated drug and reduce the drug release effectively. Moreover, the thermal-sensitivity of aliphatic PUA and pH-sensitivity of alginate matrix would preserve after the biomineralization process.Graphical AbstractHighlights► Biomimetic alginate/CaCO3 membranes were prepared under compressed CO2. ► Aliphatic PUA was employed as the thermal-responsive composition. ► The interaction between PAA and PUA contributed the formation of CaCO3. ► The release profile was sustained with the introducing of CaCO3. ► Drug release behaviors were pH- and thermal- responsive.
Co-reporter:Jun Shi;Chao Du;Jin Shi;Yaming Wang
Macromolecular Bioscience 2013 Volume 13( Issue 4) pp:494-502
Publication Date(Web):
DOI:10.1002/mabi.201200411
Co-reporter:Fuyun Pei, Yingliang Liu, Shengang Xu, Jing Lü, Chenxu Wang, Shaokui Cao
International Journal of Hydrogen Energy 2013 Volume 38(Issue 6) pp:2670-2677
Publication Date(Web):27 February 2013
DOI:10.1016/j.ijhydene.2012.12.045
The application of hydrogen energy potentially addresses energy and environmental problems. In order to improve the photocatalytic efficiency, nanocomposite of N-doped TiO2 with graphene oxide (NTG) is prepared and characterized with Fourier transform infrared spectra (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman spectra, X-ray photoelectron spectroscopy (XPS), atomic force microscope (AFM), photoluminescent spectra. The application of NTG to hydrogen evolution exhibits high photocatalytic efficiency of 716.0 or 112.0 μmol h−1 g−1 under high-pressure Hg or Xenon lamp, which is about 9.2 or 13.6 times higher than P25 photocatalyst. This is mainly attributed to the N-doping of TiO2 and the incorporation of graphene oxide resulting in narrow band gap, together with the synergistic effect of fast electron-transporting of photogenerated electrons and the efficient electron-collecting of graphene oxide retarding charge recombination. These results provide a significant theoretical foundation for the potential application of N-doping photocatalysts to hydrogen evolution.Graphical abstractHighlights► Nanocomposite of N–TiO2 with graphene oxide is prepared by hydrothermal process. ► NTG exhibits high photocatalytic efficiency in hydrogen evolution. ► Photocatalytic efficiency of NTG is improved from N-doped TiO2 and graphene oxide. ► Nitrogen-doping of TiO2 is to narrow band gap and to enhance light absorption. ► Fast electron-transporting and efficient electron-collecting is synergistic.
Co-reporter:Desheng Feng, Jun Shi, Xiaojuan Wang, Li Zhang and Shaokui Cao
RSC Advances 2013 vol. 3(Issue 47) pp:24975-24982
Publication Date(Web):17 Oct 2013
DOI:10.1039/C3RA44609C
The hybrid hydroxyapatite (HAP) hollow microparticles were achieved by combining HAP hollow microparticles and chitosan/sodium alginate (CHI/SA) multilayers via the layer-by-layer (LbL) self-assembly technique. Doxorubicin hydrochloride (DOX) loading and release investigation indicated that the prepared hybrid CHI/SA/HAP hollow microparticles with a hollow hydroxyapatite core and polymer multilayer shell exhibited high drug loading efficiency, sustained and pH-dependent drug release properties. The drug loading efficiency of CHI/SA/HAP hollow microparticles was 90.0%, which was much higher than that of solid HAP microparticles (39.6%). Compared to the solid HAP microparticles having a higher amount of released DOX over the initial 1 h (about 44.4% of total released drug over 24 h), CHI/SA/HAP hollow microparticles displayed sustained release properties with the value of only 28.4% with the same treatment. Moreover, the drug release of hybrid CHI/SA/HAP hollow microparticles was pH-dependent because of the different electrostatic interaction in the CHI/SA multilayers at different pH values and the dissolution of HAP hollow core under acidic conditions. The results indicate that the hybrid CHI/SA/HAP hollow microparticles show great potential as a novel drug carrier for controllable drug delivery.
Co-reporter:Li Zhang, Ye Li, Jun Shi, Gaoquan Shi, Shaokui Cao
Materials Chemistry and Physics 2013 Volume 142(2–3) pp:626-632
Publication Date(Web):15 November 2013
DOI:10.1016/j.matchemphys.2013.08.007
•Nonvolatile rewritable memory effect in P3HT–graphene composite is demonstrated.•The memory device was fabricated through a simple solution processing technique.•The device shows a remarkable electrical bistable behavior and excellent stability.•Memory mechanism is deduced from the modeling of the currents in both states.An electrically bistable device utilizing a nanocomposite of hexadecylamine-functionalized graphene oxide (HDAGO) with poly(3-hexylthiophene) (P3HT) is demonstrated. The device has an ITO/P3HT-HDAGO/Al sandwich structure, in which the composite film of P3HT-HDAGO was prepared by simple solution phase mixing of the exfoliated HDAGO monolayers with P3HT matrix and a spin-coating method. The memory device exhibits typical bistable electrical switching behavior and a nonvolatile rewritable memory effect, with a turn-on voltage of about 1.5 V and an ON/OFF-state current ratio of 105. Under ambient conditions, both the ON and OFF states are stable under a constant voltage stress or a continuous pulse voltage stress at a read voltage of 1 V. The conduction mechanism is deduced from the modeling of the nature of currents in both states, and the electrical switching behavior can be attributed to the electric-field-induced charge transfer between P3HT and HDAGO nanosheets.
Co-reporter:Chao Du, Jun Shi, Jin Shi, Li Zhang, Shaokui Cao
Materials Science and Engineering: C 2013 Volume 33(Issue 7) pp:3745-3752
Publication Date(Web):October 2013
DOI:10.1016/j.msec.2013.05.004
•Hybrid CaCO3 microparticles were prepared via LbL self-assembly technique.•Thermal-/pH-responsive aliphatic PUA was employed as the smart component.•The hybrid microparticles could assuage the initial burst release of DOX.•The drug release of hybrid microparticles was thermal-/pH-dual responsive.Hybrid CaCO3 microparticles coated by sodium poly(styrene sulfonate) (PSS) and aliphatic poly(urethane-amine) (PUA) were developed as thermal-/pH-responsive drug delivery vehicles via LbL self-assembly technique. The DOX release from the CaCO3 microparticles was higher than 60% within 36 h, whereas the value of PUA/PSS-coated microparticles was only 20%. The results demonstrated that the PUA/PSS multilayer coating could reduce the drug release rate and significantly assuage the initial burst release of DOX. In addition, the drug release of the hybrid microparticles was found to be thermal-/pH-dual responsive. More interestingly, more than 90% of DOX was released in 36 h at pH 2.1 and 55 °C owing to the combined action of the dissolution of the CaCO3 core and the shrinkage of aliphatic PUA.Hybrid CaCO3 microparticles coated by PSS and aliphatic PUA were developed as thermal-/pH-dual responsive drug delivery vehicles via LbL self-assembly technique.
Co-reporter:Fuyun Pei, Yingliang Liu, Li Zhang, Shengping Wang, Shengang Xu, Shaokui Cao
Materials Research Bulletin 2013 48(8) pp: 2824-2831
Publication Date(Web):
DOI:10.1016/j.materresbull.2013.04.018
Co-reporter:Lina Zou, Yinfeng Li, Shaokui Cao, Baoxian Ye
Talanta 2013 Volume 117() pp:333-337
Publication Date(Web):15 December 2013
DOI:10.1016/j.talanta.2013.09.035
•GNPs/PAn-LB GCE was constructed as voltammetric sensor for the first time.•GNPs would maintain its original state and thereby full play its electric activity.•Electrochemical behavior of EP and UA at this sensor was investigated.•Simultaneous determination of EP and UA in the sensor has better sensitivity comparing with other voltammetric sensors.•Detection of EP and UA using this sensor in human blood serum has satisfactory results.Gold nanoparticles/polyaniline nanocomposite thin film was deposited onto the surface of glassy carbon electrode(GCE) by Langmuir–Blodgett(LB) technology to fabricate a new voltammetric sensor (GNPs/PAn-LB GCE) for epinephrine(EP) and uric acid(UA) detection. Cyclic voltammetry, electrochemical impedance spectroscopy and atomic force microscopy were employed to study the characteristic of the GNPs/PAn-LB film. Electrochemical behaviors of EP and UA at the modified electrode were investigated in pH 6.6 phosphate buffer solutions. A sensitive electroanalytical method for simultaneous determination of EP and UA was proposed with high precision and good reproducibility.
Co-reporter:Jun Shi, Wenyan Qi, Gefei Li, Shaokui Cao
Materials Science and Engineering: C 2012 Volume 32(Issue 5) pp:1299-1306
Publication Date(Web):1 July 2012
DOI:10.1016/j.msec.2012.04.008
Poly(N-isopropylacrylamide) (PNIPAAm)/calcium phosphate (CaP) hybrid nanocomposites with dual-responsive controlled drug delivery property have been prepared by in-situ biomineralization process. Poly(acrylic acid) (PAA) is used as a crystal growth additive to control the morphology of the hybrid nanocomposites. The interaction between PAA and Ca2+ contributes to the formation of homogeneous and robust nanocomposites. Vitamin B2 release behavior is found to be pH- and thermal-responsive. Additionally, the release profiles are sustained with the introduction of CaP, indicating that CaP nanocrystallines could decrease the permeation of the encapsulated drug effectively. The results suggest that the prepared hybrid nanocomposites can be used as “smart” nanoscale materials for sustained dual-responsive drug delivery.PNIPAAm/CaP hybrid nanocomposites with dual-responsive sustained drug delivery property had been prepared by in-situ biomineralization process. The interaction among PNIPAAm, PAA and Ca2+ contributed the homogeneous morphology and the smart drug release property of the nanocomposites.Highlights► PNIPAAm/CaP hybrid nanocomposites were prepared by biomimetic self-assembly. ► The interaction between PAA and Ca2+ enabled the homogeneity and robustness of nanocomposite. ► Drug release behaviors were pH- and thermal-responsive. ► The release profile was sustained with the introduction of CaP.
Co-reporter:Haiyan Pei, Wei Li, Yingliang Liu, Dongfang Wang, Jin Wang, Jun Shi, Shaokui Cao
Polymer 2012 Volume 53(Issue 1) pp:138-144
Publication Date(Web):5 January 2012
DOI:10.1016/j.polymer.2011.11.018
With the aim of multifunctionalized all-optical photorefractive polymers bearing a non-conjugated main chain (NCMC), four novel norbornene-containing monomers were synthesized by introduction of different alkyl spacers between the functional chromophore and norbornene group. The polymers were prepared via ring-opening metathesis polymerization (ROMP) and characterized by IR, UV–Vis, GPC, DSC, TG, etc. Their number average molecular weights (Mn) are higher than 1.0 × 104, and their glass transition temperatures are in the range from 75 °C to 153 °C depending on the volume of functional group and spacer length. The polymers have good thermal stability up to 280 °C and excellent solubility in THF. Optically transparent films were fabricated with N-ethyl-carbazole (ECZ) as a plasticizer and C60 as a charge generator. Their photorefractive performance was evaluated at 633 nm by two-beam-coupling (TBC) experiment at a zero electrical field. TBC signals were observed from these films without prepoling, indicating that the synthesized NCMC polymers bear an all-optical photorefractive property.
Co-reporter:Yingliang Liu;Haiyan Pei;Li Zhang;Jun Shi
Macromolecular Symposia 2012 Volume 317-318( Issue 1) pp:227-239
Publication Date(Web):
DOI:10.1002/masy.201200006
Abstract
Organic all-optical photorefractive (PR) materials will soon become an interesting topic owing to the convenient signal-writing without the application of external electrical field and poling, even without any photosensitizer. In this paper, organic all-optical PR materials synthesized in our laboratory have been systematically summarized including organic monolithic PR molecular glasses with a linear or hyperbranched chemical structure such as organic carbazole/triphenylamine-based amorphous compounds, and PR polymers with a non-conjugated main chain (NCMC) such as polymethacrylates, polyphosphazenes and polynorbornenes. Much progress has been made not only in the synthesis strategy of organic all-optical materials but also in understanding the primary mechanism of all-optical PR effect in organic materials. It is believed that the outcoming of organic all-optical PR materials will broaden the application fields of organic PR materials.
Co-reporter:Gang Qin, Yuhan Song, Rui Jin, Jun Shi, Zhiyong Yu and Shaokui Cao
Green Chemistry 2011 vol. 13(Issue 6) pp:1495-1498
Publication Date(Web):14 Apr 2011
DOI:10.1039/C1GC15041C
By using ionic liquids as reaction media, gas-liquid acetylene hydrochlorination proceeded efficiently under catalysis of nonmercuric metal chlorides.
Co-reporter:Jun Shi, Zhengzheng Zhang, Gefei Li and Shaokui Cao
Journal of Materials Chemistry A 2011 vol. 21(Issue 40) pp:16028-16034
Publication Date(Web):19 Aug 2011
DOI:10.1039/C1JM11838B
Alginate/CaCO3 hybrid beads with pH- and thermal-responsive drug release properties were prepared under compressed CO2 using aliphatic poly(urethane-amine)s (PU) as the thermal-responsive component. Polyacrylic acid (PAA) was used as a crystal growth additive to control the structure of the hybrid beads. The hybrid beads were characterized by using scanning electron microscopy, X-ray powder diffraction and thermogravimetric analysis. The interaction between PAA and aliphatic PU contributed to the formation of alginate beads with a compact CaCO3 shell. Indomethacin release behaviour was found to be pH- and thermal-responsive. The release profiles were sustained with CaCO3 microparticles, indicating that the compact CaCO3 shell could hinder the permeability of the encapsulated drug and reduce the drug release effectively. The results suggest that the hybrid alginate beads can be used as “smart” polysaccharide materials for sustained dual-responsive drug delivery.
Co-reporter:Li Zhang, Shengang Xu, Zheng Yang, Shaokui Cao
Materials Chemistry and Physics 2011 Volume 126(Issue 3) pp:804-810
Publication Date(Web):15 April 2011
DOI:10.1016/j.matchemphys.2010.12.038
A novel series of triphenylamine-based photorefractive molecules M1–M5 with the different push-pull structures were designed and prepared. These molecules can form stable glasses with low glass transition temperature and their optical absorptions as well as photoconductivities at 633 nm increase systematically with increasing acceptor strength and conjugation length. As an unambiguous evidence, the two-beam-coupling experiment was performed to prove the photorefractive effect in each compound with or without an additional sensitizer. Obvious two-beam-coupling effects were obtained for the molecules with good film-forming ability and long-term stability, and among them single-component M1 which has a highly asymmetric structure using both a nitrobenzene and a cyano group as the acceptor showed the best PR performance with a gain coefficient of 52 cm−1 at 0 V μm−1 and 165 cm−1 at 40 V μm−1. Fast response time of 0.025–0.23 s were also obtained at low electric field for these glasses. The correlation of the molecular structure with the PR property was discussed, and a possible explanation for the unique energy transfer observed in M1 and M2 under zero field was proposed.Research highlights▶ A series of triphenylamine-based molecular glasses with low Tg and long-term stability were designed and prepared via simple reactions. ▶ Single-component M1 exhibited the better PR performance with a gain coefficient of 52 cm−1 (0 V μm−1) and 165 cm−1 (40 V μm−1). Fast response time of 0.025–0.23 s were obtained at low electric field for these glasses. ▶ The overall performances suggest that the present triphenylamine-based molecules are potentially good candidates for commercial application in organic photorefractive devices.
Co-reporter:Yanrong Wang, Shengang Xu, Tao Chen, Hongwu Guo, Qiongyan Liu, Baoxian Ye, Zhi Zhang, Zhiqun He and Shaokui Cao
Polymer Chemistry 2010 vol. 1(Issue 7) pp:1048-1055
Publication Date(Web):14 May 2010
DOI:10.1039/C0PY00096E
Aiming to prepare photovoltaic materials with light and thermal stability, ruthenium complexes with broad absorption in the visible region were introduced to a polyimide, bpy-PI, which contains a bipyridine ligand in each repeating unit. The chemical structures of the monomers and polymers were confirmed by 1H NMR, IR, and elemental analysis. The prepared polyimide containing ruthenium complexes (bpy-PI–Ru) showed good solubility in common organic solvents such as DMF, NMP, DMSO and DMAc. UV-vis measurements revealed that bpy-PI–Ru exhibits very broad absorptions in the range 350–750 nm due to the introduction of ruthenium complexes. Such absorption enhancement would enable the polymer to harvest solar light in the visible region. The onset oxidation potential of bpy-PI–Ru was measured as 0.68 V (vs. SCE), which is about 0.06 V lower than that of bpy-PI. The band gap of bpy-PI–Ru is 1.35 eV as measured by cyclic voltammetry. Solar cell devices were fabricated based on bpy-PI–Ru or the blend of bpy-PI–Ru and PCBM. Current density-voltage (J-V) measurement of the devices showed a typical rectifying behavior under a 55 mW cm−2 compact white arc lamp. The open-circuit voltages and short-circuit densities were measured to be in the ranges 0.19–0.52 V and 0.0015–0.38 mA cm−2, respectively. The short-circuit density could be further improved by anode modification through deposition of PEDOT:PSS on ITO surface.
Co-reporter:Jun Shi, Xiaopei Liu, Yujun Shang, Shaokui Cao
Journal of Membrane Science 2010 Volume 352(1–2) pp:262-270
Publication Date(Web):15 April 2010
DOI:10.1016/j.memsci.2010.02.026
Biomineralized polysaccharide alginate membranes with multi-responsive drug release property were prepared via a one-step method. The formation of a biomineralized polysaccharide composition in the membrane was clearly identified through scanning electron microscopy (SEM), energy dispersive X-ray spectrometer (EDS) and Fourier transform infrared spectroscopy (FT-IR). Additionally, the calcium phosphate mineralized component could be found not only in the surface but also in the cross section of the membranes. Drug release behaviours were examined by using indomethacin as a model drug, and the release profiles of the developed membrane were found to be pH-, thermo- and ionic strength-responsive. The drug release of the biomineralized polysaccharide alginate membranes was around 80% within 600 min, while that of the unmineralized ones was almost 100%. These results indicate that the biomineralized polysaccharide component can prevent the permeation of the encapsulated drug and reduce the drug release effectively. The resulting membranes can be used as “smart” polysaccharide material for sustained multi-responsive drug delivery.
Co-reporter:Shengang Xu;Yingliang Liu;Jianghui Li;Yanbin Wang
Polymers for Advanced Technologies 2010 Volume 21( Issue 9) pp:663-668
Publication Date(Web):
DOI:10.1002/pat.1487
Abstract
Two phenothiazine-based conjugated polymers, poly(3, 7-divinylene-N-octyl-phenothiazine-alt-benzo-2,1,3- thiadiazole) (PQS) and poly(3,7-divinylene-N-octyl-phenothiazine-alt-benzo-2,1,3-selenodiazole) (PQSe) were synthesized by Heck coupling reaction. The chemical structures of the two polymers were confirmed by 1H-NMR and Ft-IR. They showed good solubility in some common organic solvents such as tetrahydrofuran (THF), chloroform. The weight-average molecular weight (Mw) of the polymers determined by GPC in THF against polystyrene standards was 3.7 × 103 for PQS and 1.9 × 103 for PQSe, respectively. The temperatures of 5% weight loss (T5) were 385.0°C for PQS and 324.0°C for PQSe, respectively, determined by TGA measurements under nitrogen ambience. UV–vis absorption spectra of the polymer films showed the absorption maxima at 537 nm for PQS and 539 nm for PQSe, with the full width at half maximum (FWHM) of 190 and 230 nm, respectively. The optical band gaps () of the polymer films are 1.86 eV for PQS and 1.80 eV for PQSe, respectively. As the polymers have low-band-gap and broad absorption in the visible region, they may be used as potential light-harvesting materials for photovoltaic devices (PVDs). Furthermore, photoluminescence (PL) spectra of the polymer solutions showed the emission maxima at 698 nm for PQS and 709 nm for PQSe, with FWHM of 152 nm and 167 nm, respectively, which revealed that these two polymers may be used as red and near infrared light-emitting materials for polymeric light-emitting diodes (PLEDs). Copyright © 2009 John Wiley & Sons, Ltd.
Co-reporter:Jian-Zhuang Chen;Qiao-Ling Zhao;Hui-Chao Lu;Jin Huang;Shao-Kui Cao;Zhi Ma
Journal of Polymer Science Part A: Polymer Chemistry 2010 Volume 48( Issue 9) pp:1894-1900
Publication Date(Web):
DOI:10.1002/pola.23954
Abstract
The design and synthesis of well-defined polymethylene-b-polystyrene (PM-b-PS, Mn = 1.3 × 104–3.0 × 104 g/mol; Mw/Mn (GPC) = 1.08–1.18) diblock copolymers by the combination of living polymerization of ylides and atom transfer radical polymerization (ATRP) was successfully achieved. The 1H NMR spectrum and GPC traces of PM-b-PS indicated the successful extension of PS segment on the PM macroinitiator. The micellization behavior of such diblock copolymers in tetrahydrofuran were characterized by dynamic light scattering (DLS) and atomic force microscopy (AFM) techniques. The average aggregate sizes of PM-b-PS diblock copolymers with the same length of PM segment in tetrahydrofuran solution (1.0 mg mL−1) increases from 104.2 nm to 167.7 nm when the molecular weight of PS segment increases. The spherical precipitated aggregates of PM-b-PS diblock copolymers with an average diameter of 600 nm were observed by AFM. Honeycomb porous films with the average diameter of 3.0 μm and 6.0 μm, respectively, were successfully fabricated using the solution of PM-b-PS diblock copolymers in carbon disulfide via the breath-figure (BF) method under a static humid condition. The cross-sections of low density polyethylene (LDPE)/polystyrene (PS)/PM-b-PS and LDPE/polycarbonate (PC)/PM-b-PS blends were observed by scanning electron microscope and reveal that the PM-b-PS diblock copolymers are effective compatilizers for LDPE/PS and LDPE/PC blends. © 2010 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 48: 1894–1900, 2010
Co-reporter:L. Zhang;J. Shi;Z. W. Jiang;M. M. Huang;Z. J. Chen;Q. H. Gong;S. K. Cao
Advanced Functional Materials 2008 Volume 18( Issue 2) pp:362-368
Publication Date(Web):
DOI:10.1002/adfm.200700257
Abstract
Two hyperstructured photorefractive (PR) molecular glasses (M1 and M2) with a cyclotriphosphazene core are synthesized via nucleophilic substitution and an azo-coupling reaction. These molecules exhibit excellent solubility in common organic solvents and maintain a complete amorphous state in spite of their high glass-transition temperature. The nonlinear optical effects, two-beam coupling and four-wave mixing, respectively, are used to prove the PR performance in the optically transparent films of M1 and M2 doped with 30 % N-ethyl-carbazole. With no external electric field, a gain coefficient of 102 cm–1 and diffraction efficiency of 24 % are obtained in the composite made from M1, and an even higher gain coefficient of 214 cm–1 and diffraction efficiency of 31 % are obtained in the composite made from M2 owing to its higher chromophore loading.
Co-reporter:Jun Shi;Lihua Liu;Xiaopei Liu;Ximeng Sun
Polymers for Advanced Technologies 2008 Volume 19( Issue 11) pp:1467-1473
Publication Date(Web):
DOI:10.1002/pat.1149
Abstract
In order to obtain dual-stimuli-responsive (temperature/pH) alginate beads that exhibit LCST close to human body temperature for sustained drug release applications, poly (NIPAAm-co-AAm) hydrogel (with LCST 37.5°C) were selected and associated with calcium alginate to prepare inorganic–organic hybrid biomineralized polysaccharide alginate beads via a one-step method in this paper. Scanning electron microscopy (SEM) and energy dispersive X-ray spectrometer (EDS) results demonstrated that calcium phosphate could not only be found in the surface but also in the cross-section of biomineralized polysaccharide beads. Both equilibrium swelling and indomethacin release behavior were found to be pH- and thermo-responsive. In addition, indomethacin release profile could be sustained with a inorganic–organic hybrid membrane: the release amount reached 96% within 4 hr for the unmineralized beads, while a drug release of only 64% obtained after subjecting the biomineralized polysaccharide beads to the same treatment. These results indicate that the biomineralized polysaccharide membrane could prevent the permeability of the encapsulated drug and reduce the drug release rate effectively. The studied system has the potential to be used as an effective smart sustainable delivery system for biomedical applications. Copyright © 2008 John Wiley & Sons, Ltd.
Co-reporter:Yingliang Liu;Huayu Cao;Jianghui Li;Zhijian Chen;Lixin Xiao;Qihuang Gong
Polymers for Advanced Technologies 2008 Volume 19( Issue 12) pp:1839-1843
Publication Date(Web):
DOI:10.1002/pat.1212
Abstract
An electroluminescent polymer was synthesized by Wittig condensation and characterized by the measurements of 1H-NMR, IR, gel permeation chromatography (GPC), UV–Vis, PL, and cyclic voltammetry (CV). The polymer can be dissolved in common organic solvents such as tetrahydrofuran (THF), chloroform, and dichloromethane. The electroluminescent investigation showed that the non-doped devices with a double-layer configuration (ITO/PEDOT:PSS/Polymer/Mg:Ag) have a stable green emission property. The maximum luminance of the annealed device reaches 2317 cd/m2. The emission maximum and the CIE 1931 coordinate values are respectively stabilized at 552 nm and near (x, y) = (0.43, 0.55) with different voltages. Copyright © 2008 John Wiley & Sons, Ltd.
Co-reporter:Yingliang Liu;Huayu Cao;Yuanrong Xin;Jianghui Li;Zhijian Chen;Qihuang Gong
Polymers for Advanced Technologies 2008 Volume 19( Issue 8) pp:1084-1091
Publication Date(Web):
DOI:10.1002/pat.1083
Abstract
A conjugated polymer with a carbazole moiety, poly(3,6-divinylene-N-octyl-carbazole-p-phenylene), was synthesized by Wittig reaction. The polymer can be dissolved in common organic solvents such as THF, chloroform, etc. Using this polymer as an active layer, single-layer non-doped PLEDs with different thicknesses were fabricated by a spin-coating approach. The results suggested that electroluminescence spectra are changed with the film thickness of the polymer emitter. Fortunately, CIE 1931 coordinate values are moved to the white-light region only by changing the film thickness. Copyright © 2008 John Wiley & Sons, Ltd.
Co-reporter:Yingliang Liu;Shengang Xu;Jianghui Li;Yuanrong Xin;Guoxin Zhao;Baoxian Ye
Polymers for Advanced Technologies 2008 Volume 19( Issue 7) pp:793-800
Publication Date(Web):
DOI:10.1002/pat.1036
Abstract
Two series of conjugated polymers with a carbazole moiety were synthesized by Knovenagel and Wittig condensations. The chemical structure, thermogravimetric, photophysical and electrochemical properties of the polymers were characterized by 1H-NMR, IR, GPC, TG, UV-vis, FL, and CV. The results indicated that PBM is the most thermally stable one and PBP is the most thermally instable one. The absorption and emission properties of the polymers were adjusted by the modification of chemical structures. The quenching effect of cyano group and oxygen atom results in the lower fluorescence quantum efficiency. The fitted emission spectra suggested that the emission spectra of all the polymers come from different vibronic transitions and aggregation emission. Copyright © 2008 John Wiley & Sons, Ltd.
Co-reporter:Shengang Xu;Yingliang Liu
Macromolecular Symposia 2008 Volume 270( Issue 1) pp:161-170
Publication Date(Web):
DOI:10.1002/masy.200851019
Abstract
Novel conjugated polymers containing carbazole, phenothiazine or triphenylamine units in the main chain were designed and synthesized via Wittig, Knovenagel or Heck condensations respectively. A majority of them have good solubility in common organic solvents, high thermal stability and good hole-injection ability. Their diluted solutions in THF showed strong absorption with the absorption maximum in the range of 294∼470 nm and the optic band gaps located in the range of 1.90∼2.75 eV. When irradiated by ultraviolet or visible light, the diluted solutions in THF of the polymers emitted light from purple to yellow color with the emission maximum in the range of 347∼597 nm and the full width at half maximum located in the range of 59∼119 nm. Several polymeric light-emitting diodes (PLEDs) devices were fabricated using these polymers as light-emitting materials, and a double-layer device composed of ITO/PEDOT:PSS/PQTN/Mg:Ag showed a good performance, in which the maximum brightness was measured as 2434.0 cd/m2 under a 11.0 V forward bias voltage. Photovoltaic devices were also investigated using these polymers as an active layer, and a device composed of ITO/PNB/PTCDI-C13/Al showed a good performance, which was estimated to have external quantum efficiency at around 1% at 330 nm. From these preliminary experimental results, we may infer that these polymers are good light-emitting materials for PLEDs; while for photovoltaic applications, their absorption spectra need to be further improved to match the solar illumination.
Co-reporter:Yingliang Liu;Huayu Cao;Jianghui Li;Zhijian Chen;Bo Qu;Qihuang Gong;Shengang Xu
Polymers for Advanced Technologies 2006 Volume 17(Issue 6) pp:468-473
Publication Date(Web):27 JUL 2006
DOI:10.1002/pat.728
Several conjugated polymers containing phenothiazine moieties in the main chain were synthesized by Knovenagel or Wittig condensations. The polymers were identified and characterized by 1H-NMR, IR, gel permeation chromatography (GPC), thermogravimetric analysis (TGA), UV-vis and fluorescent (FL) spectra. Results indicated that the m-polymer, which was prepared from the polycondensation of N-octyl-3,7-diformylphenothiazine with m-phenylene diacetonitrile, is the most thermally stable one in all the polymers synthesized. While, the p-polymer, which was prepared from the polycondensation of N-octyl-3,7-diformylphenothiazine with p-phenylene diacetonitrile, is the most thermally instable one. The introduction of a cyano group made the absorption and emissive maxima red-shift from 429 and 537 nm for the Ph-polymer to 465 and 597 nm for the p-polymer respectively. The quinoid structure formation allows the p-polymer to have a lower band gap than any other polymers. Emissive spectra of all these polymers in tetrahydrofuran (THF) solution have a narrow half-peak width. Copyright © 2006 John Wiley & Sons, Ltd.
Co-reporter:Yingliang Liu, Cong-an Di, Yuanrong Xin, Gui Yu, Yunqi Liu, Qingguo He, Fenglian Bai, Shengang Xu, Shaokui Cao
Synthetic Metals 2006 Volume 156(11–13) pp:824-827
Publication Date(Web):1 June 2006
DOI:10.1016/j.synthmet.2006.04.011
A carbazole compound was synthesized by Knovenagel condensation and characterized by the measurements of 1H NMR, IR and melting point. A multilayer organic light-emitting diode (OLED) using this compound as an active layer was fabricated by vacuum-deposition. This OLED showed a turn-on voltage of approximately 4.5 V and a maximum luminance of 910 cd/m2. Additionally, the maximum luminous efficiency was found as 0.95 cd/A, at this point the device luminance was measured as 146 cd/m2 at an operating voltage of 7 V. The coordinate value of CIE 1931 was calculated as (x, y) = (0.3843, 0.5345) from the electroluminescence (EL) spectrum, which suggested that the device can emit a yellow-green light.
Co-reporter:Yingliang Liu;Yuanrong Xin;Shengang Xu;Fenglian Bai
Polymers for Advanced Technologies 2006 Volume 17(Issue 3) pp:199-203
Publication Date(Web):6 APR 2006
DOI:10.1002/pat.715
The formation of a cylinder-like helical conformation induced by solvation was observed from a conjugated polymer poly(N-octylcarbazole ethylene). The polymer was synthesized by McMurry condensation using N-octyl-3,6-diformylcarbazole as monomer, in which the alkylcarbazolyl group was functioned as a turn angle. IR analysis indicated that the double bond in the polymer chain mainly takes a cis- conformation. Computer simulation revealed that the polymer could form into a hollow tubular nano-structure with a cavity of less than 1 nm in diameter by folding its strand. The helical conformation formed by solvent induction was further proved by the measurements of circular dichroism (CD) spectrum, specific rotatory power and fluorescent (FL) spectra. Copyright © 2006 John Wiley & Sons, Ltd.
Co-reporter:Shengang Xu;Mujie Yang;Yuxia Jin;Fenglian Bai
Polymers for Advanced Technologies 2006 Volume 17(Issue 7‐8) pp:556-561
Publication Date(Web):9 AUG 2006
DOI:10.1002/pat.753
Two series of novel ternary copolyimides containing perylene and fluorene units in the backbone were synthesized by one-step polycondensation of diamine (4,4′-(9H-fluoren-9-ylidene)bisphenylamine, FBPA) with perylene dianhydride (3,4,9,10-perylenetetracarboxylic dianhydride, PTCDA) and a comonomer [4,4′-(hexafluoroisopropylidene) diphthalic anhydride, 6FDA or 3,3′,4,4′-benzophenonetetracarboxylic dianhydride, BDTA]. The polymers were named as PFFx (PTCDA-FBPA-6FDA) and PFBx (PTCDA-FBPA-BTDA), respectively, and their chemical structures were identified by FT-IR spectra and elemental analyses. Perylene contents in the copolyimides were determined through a quantitative UV-vis spectroscopy method, which are in agreement with the values calculated from the added raw materials both for PFFx and PFBx. Gel permeation chromatography (GPC) measurement suggested that the weight average molecular weight (Mw) is in the range 2.1–5.09 × 104 and the molecular weight distribution (MWD) is 1.86–2.72 for PFFx, and those for PFBx are 2.64–4.73 × 104 and 2.44–2.92, respectively. Thermogravimetric analysis (TGA) measurements showed that the copolyimides are very thermally stable with a temperature of 10% weight loss (T10) in the range 546–563°C for PFFx, and 538–548°C for PFBx. The copolyimides also have good solubility in common organic solvents such as chloroform and tetrahydrofuran. These unique properties can be attributed to the existence of the bulky diphenylfluorene moieties in the polymer backbone. All the copolyimides can emit strong fluorescence both in solution and in films, which make them possibly be used as thermostable light-emitting materials for organic light-emitting diodes. Copyright © 2006 John Wiley & Sons, Ltd.
Co-reporter:Jun Shi, Maomao Huang, Yuanrong Xin, Zhijian Chen, Qihuang Gong, Shengang Xu, Shaokui Cao
Materials Letters 2005 Volume 59(Issue 17) pp:2199-2203
Publication Date(Web):July 2005
DOI:10.1016/j.matlet.2005.02.066
A series of monolithic photorefractive molecules forming organic glasses with low glass transition temperature (−2–69 °C) was synthesized starting from 9-(2-ethyl-hexyl)-carbazole. These molecules show distinct photoconductivity due to the carbazole moiety and obvious optical nonlinearity owing to the push–pull structure. Some of these molecules can form transparent films with good stability and excellent optical quality. The absorption of the molecules is more or less red-shifted depending on the strength of the donor–acceptor internal charge transfer. A molecule with a highly asymmetric structure using both a nitrobenzene and a cyano group as the electron-withdrawing components (M2) shows the best photorefractive performance, its gain coefficient was measured as high as 266 cm−1 at an applied electric field of 42 V/μm without any extra sensitizer while the FWM efficiency was measured to be 5% at electric fields of 27 V/μm.
Co-reporter:Yingliang Liu, Yuanrong Xin, Jianghui Li, Guoxin Zhao, Baoxian Ye, Shengang Xu, Shaokui Cao
Reactive and Functional Polymers (March 2007) Volume 67(Issue 3) pp:253-263
Publication Date(Web):March 2007
DOI:10.1016/j.reactfunctpolym.2006.12.003
Co-reporter:Jincheng Tong, Li Zhang, Fei Li, Mingming Li and Shaokui Cao
Physical Chemistry Chemical Physics 2015 - vol. 17(Issue 36) pp:NaN23537-23537
Publication Date(Web):2015/08/14
DOI:10.1039/C5CP04057D
Graphitic carbon nitride (g-C3N4) nanosheets with large aspect ratios were fabricated from bulk g-C3N4 through an efficient top-down approach of moderate disintegration–exfoliation using diluted H2SO4 as an “efficient knife”. By prior disintegration in a diluted H2SO4 solution, the exfoliation of bulk g-C3N4 was effectively accelerated. The as-prepared g-C3N4 nanosheets possess a two-dimensional (2D) thin-layer structure with seven-atom thickness, a large lateral size of about 1 μm, and a high specific surface area of 80 m2 g−1. Compared with the bulk precursor, the g-C3N4 nanosheets showed much higher efficiency of photogenerated charge transfer and separation, and consequently exhibited enhanced photocatalytic activity toward hydrogen evolution and pollutant decomposition under both full-sunlight and visible-light irradiation.
Co-reporter:Jing Wei, Jun Shi, Qiong Wu, Liu Yang and Shaokui Cao
Journal of Materials Chemistry A 2015 - vol. 3(Issue 41) pp:NaN8169-8169
Publication Date(Web):2015/09/01
DOI:10.1039/C5TB01268F
Hybrid hydroxyapatite (HAP) microparticles with a hollow HAP core and a chitosan/hyaluronic acid (CHI/HA) multilayer shell were fabricated via the hydrothermal method and the layer-by-layer (LbL) self-assembly technique. Depending on the hydrothermal reaction time, the thickness of the HAP shell could be controlled and the size of the hybrid hollow microparticles varied between 850 nm and 2 μm. The size and HAP shell thickness significantly affect the drug release property of the resulting hybrid microparticles. The DOX release results demonstrated that CHI/HA multilayers could potentially assuage the initial burst release of drug from the porous HAP matrix because the polymer multilayer shell acted as a barrier to control the exchange of the drug. In addition, the drug release of hollow hybrid HAP microparticles was pH-dependent because of the different electrostatic interaction in the CHI/HA multilayers at different pH values and the dissolution of the HAP hollow core under acidic conditions. The present paper provides a facile and green route for the fabrication of hierarchical hybrid drug carriers with controllable size, wall thickness and drug release properties by combining natural polyelectrolytes and hollow HAP microparticles, which is highly attractive for controllable drug delivery.
Co-reporter:Shuhan Xu, Jun Shi, Desheng Feng, Liu Yang and Shaokui Cao
Journal of Materials Chemistry A 2014 - vol. 2(Issue 38) pp:NaN6507-6507
Publication Date(Web):2014/07/30
DOI:10.1039/C4TB01066C
In this study, hollow hierarchical hydroxyapatite (HAP)/Au/polyelectrolyte hybrid microparticles with a hollow HAP core and polymer multilayer/Au nanoparticle (AuNPs) shell for multi-responsive drug delivery have been prepared via a layer-by-layer (LbL) technique. Thermal-/pH-dual responsive aliphatic poly(urethane-amine) (PUA) was employed as the smart component. The aggregated AuNPs inside hybrid microparticles could potentially obstruct the diffusion of doxorubicin hydrochloride (DOX) from the hollow microparticles and assuage the initial burst release of DOX. Upon irradiation with near-infrared (NIR) laser, AuNP aggregates can effectively convert light to heat and result in the rapid release of DOX due to the partial collapse of the polyelectrolyte multilayers (PUA/sodium poly(styrenesulfonate) (PSS)). In addition, due to the dissolution of HAP in the acidic media and the shrinkage of aliphatic PUA above its lower critical solution temperature (LCST), the drug release of hollow hybrid carriers exhibits distinguished pH- and thermal-dependent properties. The results indicate that the hollow HAP/Au/PUA/PSS hybrid microparticles show great potential as novel smart drug carriers for controllable drug delivery.
Co-reporter:Jun Shi, Zhengzheng Zhang, Gefei Li and Shaokui Cao
Journal of Materials Chemistry A 2011 - vol. 21(Issue 40) pp:NaN16034-16034
Publication Date(Web):2011/08/19
DOI:10.1039/C1JM11838B
Alginate/CaCO3 hybrid beads with pH- and thermal-responsive drug release properties were prepared under compressed CO2 using aliphatic poly(urethane-amine)s (PU) as the thermal-responsive component. Polyacrylic acid (PAA) was used as a crystal growth additive to control the structure of the hybrid beads. The hybrid beads were characterized by using scanning electron microscopy, X-ray powder diffraction and thermogravimetric analysis. The interaction between PAA and aliphatic PU contributed to the formation of alginate beads with a compact CaCO3 shell. Indomethacin release behaviour was found to be pH- and thermal-responsive. The release profiles were sustained with CaCO3 microparticles, indicating that the compact CaCO3 shell could hinder the permeability of the encapsulated drug and reduce the drug release effectively. The results suggest that the hybrid alginate beads can be used as “smart” polysaccharide materials for sustained dual-responsive drug delivery.
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