Co-reporter:Shanshan Wang;Jun Wang;Yang Li;Junyi Ji;Fengbao Zhang;Guoliang Zhang;Wenfeng Zhang
Industrial & Engineering Chemistry Research August 20, 2014 Volume 53(Issue 33) pp:13205-13209
Publication Date(Web):Publication Date (Web): August 7, 2014
DOI:10.1021/ie501448p
In this study, reduced graphene oxide was functionalized with ethylenediamine (EDA) by a simple one-pot process, using a lithium ethylenediamine derivative as a nucleophilic reagent at 50 °C for 10 h. The presence of EDA chains in graphene was identified by Fourier transform infrared spectroscopy (FTIR), electronic energy loss spectroscopy (EELS), X-ray photoelectron spectroscopy (XPS), and zeta potential. By using the simple amidation reaction of EDA modified graphene and subsequent host–guest interactions between β-cyclodextrins (β-CDs) and polymers carrying guest moieties, we also synthesized a new type of graphene-based β-CD supramolecular hydrogels. The obtained hydrogels exhibited the gel-to-sol transition by adding a competitive guest sodium adamantine carboxylate (AdCNa) or competitive host α-CD.
Co-reporter:Fengbao Zhang;Yang Li;Guoliang Zhang;Danyun Xu;Ping Du;Junyang Zhang;Wenchao Peng
Industrial & Engineering Chemistry Research April 27, 2016 Volume 55(Issue 16) pp:4526-4531
Publication Date(Web):2017-2-22
DOI:10.1021/acs.iecr.6b00432
To achieve remote control over the swelling/deswelling transition, chemically exfoliated MoS2 nanosheets with photothermal properties are successfully incorporated into poly(N-isopropylacrylamide) (PNIPAM) hydrogel by in situ polymerization. Different from the conventional thermal-responsive PNIPAM hydrogel, the MoS2/PNIPAM composite hydrogel here shows a reversible volumetric change in response to near-infrared (NIR) illumination. Based on this new composite hydrogel, a microfluidic device actuated remotely by NIR laser is also demonstrated.
Co-reporter:Wenchao Peng, Yang Li, Fengbao Zhang, Guoliang Zhang, and Xiaobin Fan
Industrial & Engineering Chemistry Research April 26, 2017 Volume 56(Issue 16) pp:4611-4611
Publication Date(Web):March 29, 2017
DOI:10.1021/acs.iecr.7b00371
Photocatalysis has attracted great attention due to its useful environmental applications for hazardous pollutants degradation and sustainable hydrogen evolution. Recently, transition metal dichalcogenide (TMD) based materials have shown great potential in photocatalysis field. Due to their special two-dimensional layered structure and excellent electrochemical catalysis properties, they can be used as effective cocatalysts and supports to modify semiconductors for enhanced photocatalytic activities. By loading TMDs as cocatalysts, stable junctions could be created to facilitate the photogenerated electrons transfer. Moreover, the exposed edges of TMDs are active for hydrogen evolution or oxygen activation, thus leading to the improved performance for semiconductor/TMD composite in photocatalytic H2 evolution and pollutants degradation. This review will focus on the roles of TMDs as cocatalysts for semiconductors in photocatalytic hydrogen evolution and environmental remediation. We expect our work can provide enriched information to harvest the excellent special properties of TMDs as a platform to fabricate more efficient photocatalysts for solar energy utilization.
Co-reporter:Xifan Chen;Yuanzhi Zhu;Wenchao Peng;Yang Li;GuoLiang Zhang;Fengbao Zhang
Journal of Materials Chemistry A 2017 vol. 5(Issue 12) pp:5880-5885
Publication Date(Web):2017/03/21
DOI:10.1039/C7TA00459A
Recycling anode graphite remains a significant barrier to the recovery of used Li-ion batteries. In this study, we show that anode graphite in used lithium-ion batteries is a cheap and ideal candidate for the high yield production of high-quality graphene. Attributed to the reduced interlayer force after repeated charge–discharge cycles, the sonication assisted exfoliation efficiency of the used anode graphite can be 3 to 11 times that of natural graphite, with a highest mass yield of the dispersed graphene sheets of ∼40 wt%. Importantly, the layer numbers of most of the exfoliated graphene sheets are 1–4 , and their lateral sizes are over 1 μm. Their conductivity after annealing at moderate temperature (500 °C) is up to 9100 S m−1, and their potential application in conductive ink was also demonstrated.
Co-reporter:Zhen Li, Yuxi Pi, Danyun Xu, Yang Li, Wenchao Peng, Guoliang Zhang, Fengbao Zhang, Xiaobin Fan
Applied Catalysis B: Environmental 2017 Volume 213(Volume 213) pp:
Publication Date(Web):15 September 2017
DOI:10.1016/j.apcatb.2017.05.010
•Cu2O–MoS2/graphene composite was successfully prepared by a facile two-step process.•Cu2O–MoS2/graphene shows superior photcatalytic activity for CC bond formation.•Synergetic effects of MoS2 and graphene enhanced the catalytic activity of Cu2O.Visible light driven photoredox catalysis has considered as a sustainable and promising strategy for organic synthesis. Here we report a new composite material consisting of cuprous oxide (Cu2O) nanoparticles grown on layered molybdenum disulfide (MoS2) and graphene hybrids as a high-performance photocatalyst for CC bond formation reaction. This composite material shows superior stability and reusability. The enhanced photocatalytic activity of the novel catalyst is attributed to the synergetic effects of MoS2 and graphene as cocatalysts in the composite, in which graphene serves as an excellent electron transporter, and MoS2 nanosheets provide a source of active sites. This work would open a promising way to design and fabricate the efficient composite photocatalysts for organic synthesis.Download high-res image (103KB)Download full-size image
Co-reporter:Yuanzhi Zhu;Man Qiao;Wenchao Peng;Yang Li;Guoliang Zhang;Fengbao Zhang;Yafei Li
Journal of Materials Chemistry A 2017 vol. 5(Issue 19) pp:9272-9278
Publication Date(Web):2017/05/16
DOI:10.1039/C7TA01438D
Metal-free carbon quantum dots (CQDs) have attracted great interest, but the rapid preparation of doped CQDs with tunable optical properties is still an urgent task. Herein, we report that covalent organic frameworks (covalent triazine-based frameworks, CTF-1) with layered structures can be rapidly exfoliated and cut into N-doped CQDs. The cutting mechanism involves triazine hydrolysis and breaking the bonds between the triazines and benzene rings. Experiments and density functional theory (DFT) calculations confirm that the fluorescence of the obtained CQDs mainly originates from the intrinsic state emission induced by localized π–π* transitions, despite the contribution of the defect state emission. Due to their unique chemical structure, the CQDs could be further utilized as an efficient PL probe for detecting Hg2+. This study may open up new avenues for developing new kinds of CQDs using covalent organic frameworks as the starting materials.
Co-reporter:Xiaoquan Zhu;Xiaoyu Liang;Xintai Su
RSC Advances (2011-Present) 2017 vol. 7(Issue 61) pp:38119-38124
Publication Date(Web):2017/08/02
DOI:10.1039/C7RA06294J
A three-dimensional (3D) flower-like MoS2/TiO2 nanohybrid was synthesized via a two-step hydrothermal method. It is found that the MoS2/TiO2 nanohybrid is assembled with MoS2 nanosheets and TiO2 nanoparticles. The TiO2 nanoparticles are homogeneously dispersed on the MoS2 nanosheets. Moreover, the MoS2/TiO2 nanohybrid displays excellent electrochemical performance with a high reversible capacity of 801 mA h g−1 at a current density of 100 mA g−1 after 50 cycles. It also demonstrates outstanding rate behavior with a reversible discharge capacity of 660 mA h g−1 at a current density of 1000 mA g−1 and retains a capacity of about 760 mA h g−1 as the current density is returned back to 100 mA g−1. Compared with MoS2, the MoS2/TiO2 nanohybrid displays enhanced cycling stability and superior rate capability. The excellent electrochemical performance may be attributed to the favorable synergistic effect between MoS2 and TiO2. The TiO2 particles may enhance the structure stability and shorten the transport distance of ions across the surface.
Co-reporter:Xiaobin Fan; Pengtao Xu; Yuguang C. Li; Dekai Zhou; Yifan Sun; Minh An T. Nguyen; Mauricio Terrones;Thomas E. Mallouk
Journal of the American Chemical Society 2016 Volume 138(Issue 15) pp:5143-5149
Publication Date(Web):March 31, 2016
DOI:10.1021/jacs.6b01502
The controlled exfoliation of transition metal dichalcogenides (TMDs) into pristine single- or few-layer nanosheets remains a significant barrier to fundamental studies and device applications of TMDs. Here we report a novel strategy for exfoliating crystalline MoS2 into suspensions of nanosheets with retention of the semiconducting 2H phase. The controlled reaction of MoS2 with substoichiometric amounts n-butyllithium results in intercalation of the edges of the crystals, which are then readily exfoliated in a 45 vol % ethanol–water solution. Surprisingly, the resulting colloidal suspension of nanosheets was found (by electron microscopy and atomic force microscopy) to consist mostly of trilayers. The efficiency of exfoliation of the pre-intercalated sample is increased by at least 1 order of magnitude relative to the starting MoS2 microcrystals, with a mass yield of the dispersed nanosheets of 11–15%.
Co-reporter:Yunfeng Cheng, Qingshan Zhao, Yang Li, Wenchao Peng, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
RSC Advances 2016 vol. 6(Issue 80) pp:76151-76157
Publication Date(Web):02 Aug 2016
DOI:10.1039/C6RA08021A
In this study, we synthesized a novel composite material (Au–TiO2–RGO) consisting of tiny gold nanoparticles (∼4.5 nm) grown on a layered titania (TiO2) and reduced graphene oxide (RGO) hybrid. After treatment with microwave and sulfuric acid, solid acid (SO42−/TiO2) was in situ formed on the surface of TiO2, and the resulting Au–SO42−/TiO2–RGO was determined as an enhanced catalyst for hydration reaction. The strong metal-support interaction (SMSI) between Au and TiO2 and the cooperative effect between Au and SO42−/TiO2 solid acid collectively account for the excellent performance. Moreover, due to the versatile RGO substrate, the catalyst could also be recycled and reused at least 5 times without obvious deactivation.
Co-reporter:Nan Tian, Zhen Li, Danyun Xu, Yang Li, Wenchao Peng, Guoliang Zhang, Fengbao Zhang, and Xiaobin Fan
Industrial & Engineering Chemistry Research 2016 Volume 55(Issue 32) pp:8726
Publication Date(Web):July 18, 2016
DOI:10.1021/acs.iecr.6b01420
Semiconductors are the low cost and recyclable photocatalysts for visible-light photoredox catalysis, which is one of the prospective ways to convert solar energy to chemical energy in organic synthesis. This study reports a new MoS2/ZnO composite for the aerobic oxidation of benzyl halides under visible light. Despite the limited intrinsic activity of the ZnO alone, we found that the introduction of a small amount of MoS2 nanosheets (4 wt %) could significantly improve the catalytic performances of the ZnO in visible-light photoredox catalysis.
Co-reporter:Ping Du, Yuanzhi Zhu, Junyang Zhang, Danyun Xu, Wenchao Peng, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
RSC Advances 2016 vol. 6(Issue 78) pp:74394-74399
Publication Date(Web):05 Aug 2016
DOI:10.1039/C6RA10170D
Conversion of solar energy to hydrogen requires efficient, low-cost and earth-abundant H-producing photocatalysts. Herein, a novel noble metal-free photocatalyst 1T–MoS2/CdS NRs was prepared via a simple method. The 1T–MoS2/CdS NRs hybrid showed the highest photocatalytic activity when the optimized weight ratio of metallic 1T–MoS2 to CdS NRs is 10 wt% in a lactic acid solution under visible light. A 794.93 μmol h−1 H2 evolution rate of the 1T–MoS2/CdS NRs hybrid reached not only 35 times improvement than pure CdS NRs but also 4.5 times enhancement than the 2H–MoS2/CdS NRs hybrid. The relative mechanism has been investigated. 1T–MoS2/CdS NRs interfaces could form ohmic contact with very low contact resistances to promote photoexcited electron transfer, which was different from the p/n junction on the 2H–MoS2/CdS NRs hybrid.
Co-reporter:Xiaobin Fan, Guoliang Zhang and Fengbao Zhang
Chemical Society Reviews 2015 vol. 44(Issue 10) pp:3023-3035
Publication Date(Web):17 Mar 2015
DOI:10.1039/C5CS00094G
Scientific interest in graphene as a catalyst and as a catalyst support in heterogeneous catalytic reactions has grown dramatically over the past several years. The present critical review summarizes the multiple roles of graphene in heterogeneous catalysis and highlights the influence of defects, heteroatom-containing functionalities, and graphene's two-dimensional structure on catalytic performance. We first discuss the role and advantages of graphene as a catalyst support, with emphasis on its interactions with the catalytic phases and the influence of mass transfer processes. We then clarify the origin of the intrinsic catalytic activity of graphene in heterogeneous catalytic reactions. Finally we suggest challenges and potential practical applications for graphene in industrial processes.
Co-reporter:Junyi Ji;Yang Li;Wenchao Peng;Guoliang Zhang;Fengbao Zhang
Advanced Materials 2015 Volume 27( Issue 36) pp:5264-5279
Publication Date(Web):
DOI:10.1002/adma.201501115
The increasing demand for energy has triggered tremendous research effort for the development of high-performance and durable energy-storage devices. Advanced graphene-based electrodes with high electrical conductivity and ion accessibility can exhibit superior electrochemical performance in energy-storage devices. Among them, binder-free configurations can enhance the electron conductivity of the electrode, which leads to a higher capacity by avoiding the addition of non-conductive and inactive binders. Graphene, a 2D material, can be fabricated into a porous and flexible structure with an interconnected conductive network. Such a conductive structure is favorable for both electron and ion transport to the entire electrode surface. In this review, the main processes used to prepare binder-free graphene-based hybrids with high porosity and well-designed electron conductive networks are summarized. Then, the applications of free-standing binder-free graphene-based electrodes in energy-storage devices are discussed. Future research aspects with regard to overcoming the technological bottlenecks are also proposed.
Co-reporter:Qingshan Zhao, Yuanzhi Zhu, Zhen Sun, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2015 vol. 3(Issue 6) pp:2609-2616
Publication Date(Web):02 Dec 2014
DOI:10.1039/C4TA05205F
In this study, we develop a facile strategy to combine an organic amine with a palladium complex on graphene oxide (GO) as a cooperative catalyst for Tsuji–Trost allylation. A tertiary amine and palladium–diamine complex are simultaneously immobilized on a GO support through silylation and further in situ coordination processes. PdCl2 is employed as the palladium precursor, with no necessity for extra coordination ligands. Various characterizations confirm the successful preparation of the cooperative supported catalyst (GO–NEt2–2N–Pd). Systematic investigation reveals the immobilized palladium–diamine complex (GO–2N–Pd) with very low Pd loading is effective for Tsuji–Trost allylation, and incorporation of the tertiary amine shows a significant promoting effect towards the catalytic activity. GO–NEt2–2N–Pd can be readily recovered and recycled several times without reduction of its efficiency. Its excellent performance should be ascribed to synergistic catalysis effect, excellent support properties, and robust immobilization interaction.
Co-reporter:Zhen Li, Wenfeng Zhang, Qingshan Zhao, Hanying Gu, Yang Li, Guoliang Zhang, Fengbao Zhang, and Xiaobin Fan
ACS Sustainable Chemistry & Engineering 2015 Volume 3(Issue 3) pp:468
Publication Date(Web):January 26, 2015
DOI:10.1021/sc5006654
A visible-light photoredox with homogeneous catalyst-like transition metal complexes and organic dyes shows promising applications in organic synthesis. However, the practical applications of these photocatalysts are hampered by the difficulty of separating and recycling them from the reaction mixtures. In this study, we report the covalent immobilization of Eosin Y on reduced graphene oxide and demonstrate the obtained hybrid can be used as a recyclable photocatalyst with excellent catalytic performances in the aerobic oxidation of α-aryl halogen derivatives.Keywords: covalent immobilization; Eosin Y; graphene; metal-free; Photocatalysis
Co-reporter:Xiaojie Li, Jun Wang, Danyun Xu, Zhen Sun, Qingshan Zhao, Wenchao Peng, Yang Li, Guoliang Zhang, Fengbao Zhang, and Xiaobin Fan
ACS Sustainable Chemistry & Engineering 2015 Volume 3(Issue 5) pp:1017
Publication Date(Web):April 15, 2015
DOI:10.1021/acssuschemeng.5b00182
Visible light photoredox catalysis has been demonstrated to be a promising and green strategy for organic synthesis. In this study, a nanocomposite of PbBiO2Br nanoparticles and NbSe2 nanosheet was prepared as a high performance photocatalyst for the visible light-driven asymmetric alkylation of aldehyde. It was found that the introduction of a small amount of NbSe2 (0.5 wt %) to the PbBiO2Br semiconductor could result in ∼50% increase in the yield of the final product. This study shows that NbSe2 nanosheets can be used as an efficient support to suppress the recombination of photoinduced electron–hole pairs and contribute to the enhanced photocatalytic performances of semiconductors in the visible light-driven catalysis.Keywords: Asymmetric alkylation; NbSe2; Organic synthesis; Photocatalysis; Two-dimensional nanosheet;
Co-reporter:Zhen Sun, Qingshan Zhao, Guanghui Zhang, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
RSC Advances 2015 vol. 5(Issue 14) pp:10352-10357
Publication Date(Web):07 Jan 2015
DOI:10.1039/C4RA13575J
Au–Pd bimetallic nanoparticles (NPs) with core–shell structures have been successfully anchored on chemical exfoliated MoS2 (Au–Pd/MoS2) through a facile co-reduction method at room temperature. The Au–Pd/MoS2 hybrids were characterized by X-ray diffraction (XRD), scanning electronic microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), energy dispersive X-ray spectroscopy (EDX) and X-ray photoelectron spectroscopy (XPS). The pristine MoS2 nanosheets exhibit some peroxidase-like activity for the oxidation of 3,3,5,5-tetramethylbenzidine (TMB), and their catalytic activity is significantly enhanced by the deposition of Au–Pd NPs. A systematic study revealed that Au–Pd NPs with a mass ratio of 1:2 on MoS2 (Au1.0Pd2.0/MoS2) showed the highest catalytic activity compared with other counterparts. This excellent performance of the Au1.0Pd2.0/MoS2 hybrids should be ascribed to not only the intrinsic catalytic activity of MoS2, but also the complicated metal–metal and metal–support interactions.
Co-reporter:Wenfeng Zhang, Hanying Gu, Zhen Li, Yuanzhi Zhu, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2014 vol. 2(Issue 26) pp:10239-10243
Publication Date(Web):29 Apr 2014
DOI:10.1039/C4TA01446D
In this study, a bifunctional graphene oxide material (GO–AEP–UDP) with a general acid, the ureidopropyl (UDP) group, and a general base, the 3-[2-(2-aminoethylamino)ethylamino]-propyl (AEP) group, was synthesized by silylanization of graphene oxide (GO) with organoalkoxysilane precursors. Characterization of the obtained GO–AEP–UDP was carried out by Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and zeta potential measurements. Systematic studies demonstrated that GO–AEP–UDP has superior catalytic performance in the classic Henry reaction of 4-nitrobenzaldehyde with nitromethane. It was found that the relative concentration and spatial arrangement of cooperative functional groups were very important factors in the synergistic catalysis.
Co-reporter:Jun Wang, Jingwen Ma, Xiaojie Li, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Chemical Communications 2014 vol. 50(Issue 91) pp:14237-14240
Publication Date(Web):25 Sep 2014
DOI:10.1039/C4CC06869F
Mesoporous Cu2O spheres with a large pore size (LP-Cu2O) bring out a better performance towards the photocatalytic aza-Henry reaction than Cu2O spheres with a small pore size (SP-Cu2O). This work highlights the internal diffusion coefficient as a critical parameter for the fabrication of porous photocatalysts.
Co-reporter:Miao Zhang, Danyun Xu, Junyi Ji, Yuhong Wang, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
RSC Advances 2014 vol. 4(Issue 37) pp:19226-19228
Publication Date(Web):14 Apr 2014
DOI:10.1039/C4RA01474J
We demonstrated a facile borane hydrogenation route to hydrogenate reduced graphene oxide (RGO). This strategy is simple and might be scaleable for mass production of partially hydrogenated RGO with a band gap of ∼1.8 eV.
Co-reporter:Wenfeng Zhang, Qingshan Zhao, Tong Liu, Yuan Gao, Yang Li, Guoliang Zhang, Fengbao Zhang, and Xiaobin Fan
Industrial & Engineering Chemistry Research 2014 Volume 53(Issue 4) pp:1437-1441
Publication Date(Web):December 27, 2013
DOI:10.1021/ie403393u
In this study, phosphotungstic acid immobilized on amine-grafted graphene oxide (GOAP) was prepared successfully by silylanization and electrostatic interaction. The obtained GOAP was characterized by Raman spectroscopy, scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), high-resolution transmission electron microscopy (HRTEM), zeta potential measurements, and X-ray photoelectron spectroscopy (XPS). Systematic studies demonstrated that GOAP had excellent catalytic activities and robustness in the one-pot tandem deacetalization–nitroaldol reaction. The key role of the acid/base ratio in the catalytic performance of this bifunctional catalyst was also revealed by preliminary kinetic studies. This bifunctional catalyst might find promising applications in green chemistry, as it can not only reduce costs and waste by saving separation/purification steps and solvents/reagents, but also increase the yield by avoiding the separation of intermediate products.
Co-reporter:Guanghui Zhang, Jingwen Ma, Jun Wang, Yang Li, Guoliang Zhang, Fengbao Zhang, and Xiaobin Fan
Industrial & Engineering Chemistry Research 2014 Volume 53(Issue 51) pp:19878-19883
Publication Date(Web):December 4, 2014
DOI:10.1021/ie503596j
Graphene oxide (GO) has shown promising applications as supports for heterogeneous catalysts. This study reports the functionalization of GO by (3-mercaptopropyl) trimethoxysilane to immobilize lipase. The immobilization is carried out by the site-specific covalent binding between thiol groups of lipase and thiolsulfonate groups on modified GO. For the hydrolysis of p-nitrophenylpalmitate, the obtained GO–lipase shows catalytic performance (93.4%) comparable with that of the free lipase, and the reusability after 10 times is 69.9%. Compared with the free lipase, the GO–lipase exhibits good pH, thermal, and storage stability, which are important in practical applications.
Co-reporter:Qingshan Zhao, Chan Bai, Wenfeng Zhang, Yang Li, Guoliang Zhang, Fengbao Zhang, and Xiaobin Fan
Industrial & Engineering Chemistry Research 2014 Volume 53(Issue 11) pp:4232-4238
Publication Date(Web):2017-2-22
DOI:10.1021/ie500017z
Immobilization of metal complexes on solid supports is an efficient approach to remedy the drawbacks of homogeneous catalysis. In this study, an in situ strategy of synthesis and immobilization of a copper (salen) complex onto graphene oxide (GO) support has been developed. To provide the salen ligands, GO was covalently modified with an aminosilane, followed by condensation with salicylaldehyde. The copper (salen) complex was subsequently synthesized and simultaneously immobilized onto the GO surface with a designed tetrahedral chelate structure. The immobilized copper (salen) complex [Cu(salen)–f–GO] kept the two-dimensional sheetlike character of GO and was demonstrated to be highly effective for the epoxidation of olefins. It could be readily reused for successive twelve times without discernible activity and selectivity deterioration, which displays potential for practical applications.
Co-reporter:Chan Bai;Qingshan Zhao;Yang Li;Guoliang Zhang;Fengbao Zhang
Catalysis Letters 2014 Volume 144( Issue 9) pp:1617-1623
Publication Date(Web):2014 September
DOI:10.1007/s10562-014-1299-0
A graphene supported palladium (Pd) catalyst for Suzuki coupling reaction has been successfully prepared by immobilizing Pd(II) onto graphene oxide surface through the in situ coordination interaction with aminosilane ligand spacers. This catalyst showed high catalytic activities in the Suzuki coupling of various aryl halides and phenylboronic acid. Moreover, it could be readily recycled and reused for several times without discernible loss of its catalytic activity.
Co-reporter:Qingshan Zhao, Dafa Chen, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Nanoscale 2013 vol. 5(Issue 3) pp:882-885
Publication Date(Web):06 Dec 2012
DOI:10.1039/C2NR33290F
Rhodium complexes can be homogeneously immobilized on functionalized graphene oxide through coordination interaction. The obtained catalyst can be readily recycled and shows enhanced activity in the catalytic hydrogenation of cyclohexene.
Co-reporter:Wenfeng Zhang, Shanshan Wang, Junyi Ji, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Nanoscale 2013 vol. 5(Issue 13) pp:6030-6033
Publication Date(Web):23 Apr 2013
DOI:10.1039/C3NR01323E
In this study, primary and tertiary amine bifunctional graphene oxide (GO–NH2–NEt2) was prepared by silylanization of graphene oxide (GO) with amine-terminal silanes. The obtained GO–NH2–NEt2 was characterized by infrared spectrum (FTIR), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), high-resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectroscopy (XPS). Systematic studies demonstrated the GO–NH2–NEt2 had excellent catalytic activities and 100% selectivity in the classic trans-β-nitrostyrene forming reaction.
Co-reporter:Junjie Qi, Weipeng Lv, Guanghui Zhang, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Nanoscale 2013 vol. 5(Issue 14) pp:6275-6279
Publication Date(Web):29 Apr 2013
DOI:10.1039/C3NR00395G
We have successfully developed a unique graphene-based smart catalytic system which consists of the graphene supported Au–Pt bimetallic nanocatalyst with a well-defined core–shell structure and a dextran-based temperature-responsive polymer. The unique catalytic system possesses excellent catalytic performances and the catalytic activities could be readily switched on or off at different temperature windows.
Co-reporter:Qingshan Zhao, Yang Li, Ru Liu, Ao Chen, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2013 vol. 1(Issue 47) pp:15039-15045
Publication Date(Web):03 Oct 2013
DOI:10.1039/C3TA13378H
Graphene oxide (GO) is a promising support for anchoring homogeneous metal complexes because of its two-dimensional structure, huge surface area and diversity for chemical functionalizations. In this study, a ruthenium supported catalyst has been synthesized by covalently bonding a ruthenium complex (RuCl2(PPh3)3) onto the GO surface through coordination interaction with aminosilane ligand spacers. The supported catalyst showed enhanced catalytic performance towards hydrogenation of olefins and ketones compared with the homogeneous analogue, and it could be readily recycled and reused several times without discernible loss of its activity.
Co-reporter:Yang Yuan, Guanghui Zhang, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Polymer Chemistry 2013 vol. 4(Issue 6) pp:2164-2167
Publication Date(Web):11 Jan 2013
DOI:10.1039/C3PY21128B
Poly(amidoamine) modified graphene oxide was prepared via a grafting-from method and characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and atomic force microscopy (AFM). Evaluation of its adsorption capacity for heavy metal ions demonstrated that the poly(amidoamine) modified graphene oxide had superior adsorption ability towards heavy metal ions such as Cu2+, Zn2+, Fe3+, Pb2+ and Cr3+.
Co-reporter:Ao Chen, Junjie Qi, Qingshan Zhao, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
RSC Advances 2013 vol. 3(Issue 23) pp:8973-8977
Publication Date(Web):28 Mar 2013
DOI:10.1039/C3RA40718G
Graphene has attracted increasing attention as a support for heterogeneous catalysis. Although successful preparation and excellent catalytic performance of many graphene based nanocatalysts have been demonstrated, graphene supported nanocatalysts with turnable catalytic behaviors remain unexplored. In this study, we report a strategy to prepare a graphene supported Au nanocatalyst with thermo-sensitive catalytic behaviors. This smart catalytic system was prepared by introducing the temperature-responsive poly(N-isopropylacrylamide) (NIPAAm) and Au nanoparticles to graphene oxide (GO) through reversible addition–fragmentation chain transfer polymerization and direct co-reduction of HAuCl4. The obtained GO–NIPAAm–Au hybrid was systematically characterized and showed interesting thermo-sensitive catalytic activity in the catalytic reduction of 4-nitrophenol.
Co-reporter:Yang Li, Qingshan Zhao, Junyi Ji, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
RSC Advances 2013 vol. 3(Issue 33) pp:13655-13658
Publication Date(Web):14 Jun 2013
DOI:10.1039/C3RA41970C
Acid–base bifunctional catalysts are of particularly interest, but also present great challenges in synthesis and applications. In this study, acid–base bifunctional graphene oxide hybrids were obtained by the modification of graphene oxide (GO) through a silylation reaction and radical addition. The obtained bifunctional hybrids displayed high acid and base catalytic activities towards a typical one-pot acid–base reaction sequence called deacetalization–nitroaldol reaction.
Co-reporter:Yizhu Wang, Xiaobin Fan, Shulan Wang, Guoliang Zhang, Fengbao Zhang
Materials Research Bulletin 2013 48(2) pp: 785-789
Publication Date(Web):
DOI:10.1016/j.materresbull.2012.11.058
Co-reporter:Yang Li, Hongyu Chen, Lian Yeau Voo, Junyi Ji, Guanghui Zhang, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2012 vol. 22(Issue 30) pp:15021-15024
Publication Date(Web):28 May 2012
DOI:10.1039/C2JM32307A
Partially hydrogenated graphene was readily prepared by an interesting reaction between graphene oxide and phenylboronic acid. This partially hydrogenated graphene was employed to synthesize brominated graphene through subsequent radical hydrogen abstraction.
Co-reporter:Weipeng Lv, Junjie Qi, Wenqian Feng, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2012 vol. 22(Issue 22) pp:11290-11296
Publication Date(Web):03 Apr 2012
DOI:10.1039/C2JM30753G
A universal functionalization platform based on PNIPAAm grafted dextran smart polymers for, but not limited to, carbon and gold nanomaterials, is developed. The dextran based smart polymer contains three indispensable components: 1) dextran – to provide hydrophilicity and stability; 2) PNIPAAm – to provide stimuli-sensitivity; 3) dodecylthiocarbonothioylthio groups (or aminolysis-generated thiols) – to provide feasible functionalization through stable interactions between polymer and nanomaterials. The readily accessible distinctive versions of polymers can provide necessary and efficient interactions with a variety of nanomaterials: the unique dodecyl end groups provide the effective functionalization of SWNT and NGO in a noncovalent manner, while the AuNR can be covalently functionalized through aminolysis-generated thiols. These functionalized nanomaterials are simultaneously endowed with well-retained properties of interest, excellent stability and smart properties: they exhibit superior stability under various conditions and the absorption, fluorescent and aggregation properties can be smartly tuned by temperature and NIR light. The establishment of this general approach is an important step forward for development and wide-application of smart nanomaterials in catalysts, actuators, sensors and biomedicine.
Co-reporter:Wenqian Feng;Weipeng Lv;Junjie Qi;Guoliang Zhang;Fengbao Zhang
Macromolecular Rapid Communications 2012 Volume 33( Issue 2) pp:133-139
Publication Date(Web):
DOI:10.1002/marc.201100595
Abstract
A quadruple-responsive nanocomposite that responds to temperature, pH, magnetic field, and NIR is obtained by incorporating superparamagnetic iron oxide nanoparticles (SPIONs) and gold nanorods (AuNRs) into a dextran-based smart copolymer network. The dual-sensitive copolymer is prepared by sequential RAFT polymerization of methacrylic acid and N-isopropylacrylamide from trithiocarbonate groups linked to dextran in one pot. These functionalized nanocomposites with superior stability can respond to the four stimuli mentioned above well. As evidenced by UV–vis and TEM measurements, the temperature-induced unusual blue-shift in the longitudinal plasmon band is possibly due to the side-to-side assembly of AuNRs.
Co-reporter:Ying Chen, Wenchao Peng, Shaobin Wang, Fengbao Zhang, Guoliang Zhang, Xiaobin Fan
Dyes and Pigments 2012 Volume 95(Issue 2) pp:215-220
Publication Date(Web):November 2012
DOI:10.1016/j.dyepig.2012.03.009
Gold nanoparticles supported on three metal oxides, TiO2, Al2O3 and Fe2O3, were prepared by a modified precipitation-deposition method using urea as an additive. These catalysts were tested in chemoselective reduction of 4,4′-dinitrostilbene-2,2′-disulfonic acid to 4,4′-diaminostilbene-2,2′-disulfonic acid. Three reagents, hydrogen, carbon monoxide, and sodium formate, were employed as reductants. It was found that >94% of the nitrostilbene was transformed into the aminostilbene without the reduction of olefinic group. In addition, these catalysts exhibited stable performance after regeneration by calcination at 400 °C for 5 h. This clean approach provides a promising application for synthesis of amino substituted stilbene sulfonic acid on an industrial scale.Graphical abstractSelective production of 4,4′-diaminostilbene-2,2′-disulfonic acid (DSD) from 4,4′-dinitrostilbene-2,2′-disulfonic acid (DNS) without any olefinic group was reduced feasible by catalytic reduction over supported nano-sized gold catalysts with different hydrogen resources, which uncovers a clean synthetic approach for useful aromatic sulfonic stilbene.Highlights► Gold nanoparticles with similar average diameters were supported on three metal oxides. ► H2, CO, and HCOONa were used as clean reductants. ► Good selectivity (>94%) between nitro and olefinic group reduction was obtained. ► The catalytic activity can be restored by calcination at 400 °C.
Co-reporter:Junyi Ji, Guanghui Zhang, Hongyu Chen, Shulan Wang, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Chemical Science 2011 vol. 2(Issue 3) pp:484-487
Publication Date(Web):03 Dec 2010
DOI:10.1039/C0SC00484G
Acid catalysts are essential for various chemical reactions in the industrial hydrocarbon chemistry. Sulfonated carbon has shown promising application as a new, cheap and environmentally friendly solid acid catalyst. In this study, we prepared the sulfonated graphene acid catalyst, and it was characterized by electron microscopy, Raman spectroscopy, solid state 13C MAS NMR, energy dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS). Catalytic hydrolysis of ethyl acetate shows that the sulfonated graphene has highly catalytic activity and can be repetitively used as a water-tolerant solid acid catalyst.
Co-reporter:Weipeng Lv, Yang Wang, Wenqian Feng, Junjie Qi, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2011 vol. 21(Issue 17) pp:6173-6178
Publication Date(Web):14 Feb 2011
DOI:10.1039/C0JM04180G
We have developed a one-step method to prepare robust and smart gold nanoparticles (AuNPs) utilizing poly(N-isopropylacrylamide) (PNIPAAm)-grafted dextran (DexPNI) via a “grafting-onto” approach. Using NaBH4 as a reducing agent, and DexPNI as a nucleating and stabilizing agent, the AuNPs can be obtained at ambient temperature within a short reaction time. Different features of AuNPs, such as their morphologies, optical properties and temperature-responsive behaviours are found to be dependent on the dosage of the gold precursor. The DexPNI-stabilized AuNPs not only show excellent stability against heat, high salt concentration and extreme pH, but could also be readily redispersed after freeze-drying. UV measurements and kinetic analysis of the AuNPs-catalyzed reduction of 4-nitrophenol at different temperatures illuminated that the optical properties and catalytic activity of AuNPs are closely related to temperature. Compared with previously reported diffusion-regulated nanoreacters, our AuNPs provide a unique opportunity to control the reaction rate in an inverse temperature-responsive manner at 32–35 °C, and further switch off the reaction at temperatures higher than 35 °C. These temperature-responsive properties could be used to create a smart sensor and catalyst, acting as an optical temperature alarm and recloser when the reaction temperature accidentally goes beyond the limit value. By using monomers and colloidal precursors other than NIPAAm and HAuCl4, it will be straightforward to extend the present route to build a variety of robust and smart nanomaterials with unprecedented properties.
Co-reporter:Hongyu Chen, Yang Li, Fengbao Zhang, Guoliang Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2011 vol. 21(Issue 44) pp:17658-17661
Publication Date(Web):07 Oct 2011
DOI:10.1039/C1JM13356J
AucorePdshell (Au@Pd) bimetallic nanoparticles of sub-10 nm were successfully dispersed on graphene by a simple one step reducing method. The Au@Pd nanoparticles–graphene (Au@Pd–G) hybrids were characterized by high-resolution transmission electron microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, energy X-ray spectroscopy and electronic energy loss spectroscopy. Evaluation of their catalytic performance demonstrates the Au@Pd–G hybrids have extraordinary peroxidase activity as catalysts.
Co-reporter:Junyi Ji, Guanghui Zhang, Hongyu Chen, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2011 vol. 21(Issue 38) pp:14498-14501
Publication Date(Web):11 Aug 2011
DOI:10.1039/C1JM12970H
Graphene sheets decorated with metal/metal oxide nanoparticles are gaining increasing attention. In this study, sulfhydrylated graphene was prepared by reducing the sulfonic acid groups on sulfonated graphene to thiol groups. We evaluated its ability to anchor different metal/metal oxide nanoparticles by simply mixing the sulfhydrylated graphene with the corresponding pre-prepared metal/metal oxide nanoparticles. The sulfhydrylated graphene and its nanohybrids were characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), high-resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectroscopy (XPS). We demonstrate that the obtained sulfhydrylated graphene can act as a general platform to anchor different kinds of metal/metal oxide nanoparticles with different shapes, structures or properties through thiol–metal bonds. These novel hybrids will render graphene with additional interesting properties and potential applications.
Co-reporter:Weipeng Lv;Shuoqi Liu;Wenqian Feng;Junjie Qi;Guoliang Zhang;Fengbao Zhang
Macromolecular Rapid Communications 2011 Volume 32( Issue 14) pp:1101-1107
Publication Date(Web):
DOI:10.1002/marc.201100112
Co-reporter:Wenchao Peng, Ying Chen, Fengbao Zhang, Guoliang Zhang, and Xiaobin Fan
Journal of Chemical & Engineering Data 2011 Volume 56(Issue 5) pp:2700-2705
Publication Date(Web):March 7, 2011
DOI:10.1021/je101183u
The recovery of 4,4′-dinitrostilbene-2,2′-disulfonic acid (DNS) and 4,4′-diaminostilbene-2,2′-disulfonic acid (DSD) and the purification of 4-amino-4′-nitrostilbene-2,2′-disulfonic acid (ANSD) are important processes during their individual production. To increase the yields of DNS, DSD, and the purity of ANSD, detailed studies on the solubilities of these three stilbene sulfonic acids (SSA) are necessary. Herein, the static analytical method was used to investigate the effects of pH, temperature, and ionic strength on the solubilities of these three SSA. On the basis of the results, new processes were proposed to recover more DNS and DSD during their production. In addition, a new purification method was developed to obtain ANSD with a purity of > 99 %.
Co-reporter:Wenchao Peng, Ying Chen, Shidong Fan, Fengbao Zhang, Guoliang Zhang, and Xiaobin Fan
Environmental Science & Technology 2010 Volume 44(Issue 23) pp:9157-9162
Publication Date(Web):November 5, 2010
DOI:10.1021/es101950k
This study uses 4,4′-dinitrostilbene-2,2′-disulfonic acid (DNS) wastewater to produce paramycin (4-amino-2-hydroxybenzoic acid), an antitubercular agent and important pharmaceutical intermediate. The high concentrations of aromatic sulfonic acids contained in the wastewater, derived from a DNS production facility, have been transformed to paramycin in yields of more than 85%. This waste-disposal strategy, which combines oxidation using NaClO, reduction using iron powder, and subsequent alkaline fusion with NaOH, has been proven to be successful in dealing with ton-scale DNS wastewater. Compared with common treatment methods, which usually involve degrading the compounds, this new method recycles most of the aromatic sulfonic acids in the wastewater to produce paramycin. This effectively solves the associated environment problems associated with DNS wastewater and is also potentially profitable. The present approach could also lead to alternative solutions for dealing with other industrial wastewaters generated from oxidative coupling reactions of nitro-substituted toluenes to the corresponding substituted stilbenes.
Co-reporter:Yang Li, Xiaobin Fan, Junjie Qi, Junyi Ji, Shulan Wang, Guoliang Zhang, Fengbao Zhang
Materials Research Bulletin 2010 45(10) pp: 1413-1418
Publication Date(Web):
DOI:10.1016/j.materresbull.2010.06.041
Co-reporter:Yang Li;Junjie Qi;Junyi Ji;Shulan Wang;Guoliang Zhang
Nano Research 2010 Volume 3( Issue 6) pp:429-437
Publication Date(Web):2010 June
DOI:10.1007/s12274-010-0002-z
Graphene has been successfully modified with palladium nanoparticles in a facile manner by reducing palladium acetate [Pd(OAc)2] in the present of sodium dodecyl sulfate (SDS), which is used as both surfactant and the reducing agent. The palladium nanoparticle-graphene hybrids (Pd-graphene hybrids) are characterized by high-resolution transmission electron microscopy, atomic force microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, and energy dispersive X-ray spectroscopy. We demonstrate that the Pd-graphene hybrids can act as an efficient catalyst for the Suzuki reaction under aqueous and aerobic conditions, with the reaction reaching completion in as little as 5 min. The influence of the preparation conditions on the catalytic activities of the hybrids is also investigated.
Co-reporter:Jialei Jin, Yuanzhi Zhu, Yizhe Liu, Yang Li, Wenchao Peng, Guoliang Zhang, Fengbao Zhang, Xiaobin Fan
International Journal of Hydrogen Energy (16 February 2017) Volume 42(Issue 7) pp:
Publication Date(Web):16 February 2017
DOI:10.1016/j.ijhydene.2016.12.019
•We combined CoP nanoparticles and WS2 nanosheets for the first time.•We designed different CoP to WS2 mass ratios to optimize.•CoP/WS2 composites were prepared through a simple ultrasound method.•The designed composites have better catalytic activity than mere CoP and WS2.•The optimized composite has a low onset overpotential of 50 mV.Producing hydrogen through hydrogen evolution reaction by electrolyzing water is a great alternative to solve the energy crisis and air pollution. Earth abundant transition-metal phosphides, especially CoP, have emerged as promising hydrogen evolution reaction catalysts for recent years. Nowadays, attention is focused on combining CoP with other materials to improve its catalytic activity. Herein, in order to get better hydrogen evolution reaction catalyst, we combined CoP nanoparticles with WS2 nanosheets. Different CoP to WS2 mass ratios were set to find the best catalytic activity. CoP/WS2 composites were prepared through a simple ultrasound induced mixing method. And all the CoP/WS2 composites have enhanced hydrogen evolution reaction catalytic activity than pure CoP nanoparticles and WS2 nanosheets. Especially, the optimized CoP/WS2 composite has the lowest onset overpotential of 50 mV, the largest current density of 78 mA/cm2 at the overpotential of 300 mV, and the smallest Tafel slope of 64.63 mV/decade, indicating excellent hydrogen evolution reaction catalytic activity.Figure optionsDownload full-size imageDownload high-quality image (204 K)Download as PowerPoint slide
Co-reporter:Hongyu Chen, Yang Li, Fengbao Zhang, Guoliang Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2011 - vol. 21(Issue 44) pp:NaN17661-17661
Publication Date(Web):2011/10/07
DOI:10.1039/C1JM13356J
AucorePdshell (Au@Pd) bimetallic nanoparticles of sub-10 nm were successfully dispersed on graphene by a simple one step reducing method. The Au@Pd nanoparticles–graphene (Au@Pd–G) hybrids were characterized by high-resolution transmission electron microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, energy X-ray spectroscopy and electronic energy loss spectroscopy. Evaluation of their catalytic performance demonstrates the Au@Pd–G hybrids have extraordinary peroxidase activity as catalysts.
Co-reporter:Xifan Chen, Yuanzhi Zhu, Wenchao Peng, Yang Li, GuoLiang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2017 - vol. 5(Issue 12) pp:NaN5885-5885
Publication Date(Web):2017/03/06
DOI:10.1039/C7TA00459A
Recycling anode graphite remains a significant barrier to the recovery of used Li-ion batteries. In this study, we show that anode graphite in used lithium-ion batteries is a cheap and ideal candidate for the high yield production of high-quality graphene. Attributed to the reduced interlayer force after repeated charge–discharge cycles, the sonication assisted exfoliation efficiency of the used anode graphite can be 3 to 11 times that of natural graphite, with a highest mass yield of the dispersed graphene sheets of ∼40 wt%. Importantly, the layer numbers of most of the exfoliated graphene sheets are 1–4 , and their lateral sizes are over 1 μm. Their conductivity after annealing at moderate temperature (500 °C) is up to 9100 S m−1, and their potential application in conductive ink was also demonstrated.
Co-reporter:Weipeng Lv, Junjie Qi, Wenqian Feng, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2012 - vol. 22(Issue 22) pp:NaN11296-11296
Publication Date(Web):2012/04/03
DOI:10.1039/C2JM30753G
A universal functionalization platform based on PNIPAAm grafted dextran smart polymers for, but not limited to, carbon and gold nanomaterials, is developed. The dextran based smart polymer contains three indispensable components: 1) dextran – to provide hydrophilicity and stability; 2) PNIPAAm – to provide stimuli-sensitivity; 3) dodecylthiocarbonothioylthio groups (or aminolysis-generated thiols) – to provide feasible functionalization through stable interactions between polymer and nanomaterials. The readily accessible distinctive versions of polymers can provide necessary and efficient interactions with a variety of nanomaterials: the unique dodecyl end groups provide the effective functionalization of SWNT and NGO in a noncovalent manner, while the AuNR can be covalently functionalized through aminolysis-generated thiols. These functionalized nanomaterials are simultaneously endowed with well-retained properties of interest, excellent stability and smart properties: they exhibit superior stability under various conditions and the absorption, fluorescent and aggregation properties can be smartly tuned by temperature and NIR light. The establishment of this general approach is an important step forward for development and wide-application of smart nanomaterials in catalysts, actuators, sensors and biomedicine.
Co-reporter:Wenfeng Zhang, Hanying Gu, Zhen Li, Yuanzhi Zhu, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2014 - vol. 2(Issue 26) pp:NaN10243-10243
Publication Date(Web):2014/04/29
DOI:10.1039/C4TA01446D
In this study, a bifunctional graphene oxide material (GO–AEP–UDP) with a general acid, the ureidopropyl (UDP) group, and a general base, the 3-[2-(2-aminoethylamino)ethylamino]-propyl (AEP) group, was synthesized by silylanization of graphene oxide (GO) with organoalkoxysilane precursors. Characterization of the obtained GO–AEP–UDP was carried out by Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and zeta potential measurements. Systematic studies demonstrated that GO–AEP–UDP has superior catalytic performance in the classic Henry reaction of 4-nitrobenzaldehyde with nitromethane. It was found that the relative concentration and spatial arrangement of cooperative functional groups were very important factors in the synergistic catalysis.
Co-reporter:Junyi Ji, Guanghui Zhang, Hongyu Chen, Shulan Wang, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Chemical Science (2010-Present) 2011 - vol. 2(Issue 3) pp:NaN487-487
Publication Date(Web):2010/12/03
DOI:10.1039/C0SC00484G
Acid catalysts are essential for various chemical reactions in the industrial hydrocarbon chemistry. Sulfonated carbon has shown promising application as a new, cheap and environmentally friendly solid acid catalyst. In this study, we prepared the sulfonated graphene acid catalyst, and it was characterized by electron microscopy, Raman spectroscopy, solid state 13C MAS NMR, energy dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS). Catalytic hydrolysis of ethyl acetate shows that the sulfonated graphene has highly catalytic activity and can be repetitively used as a water-tolerant solid acid catalyst.
Co-reporter:Weipeng Lv, Yang Wang, Wenqian Feng, Junjie Qi, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2011 - vol. 21(Issue 17) pp:NaN6178-6178
Publication Date(Web):2011/02/14
DOI:10.1039/C0JM04180G
We have developed a one-step method to prepare robust and smart gold nanoparticles (AuNPs) utilizing poly(N-isopropylacrylamide) (PNIPAAm)-grafted dextran (DexPNI) via a “grafting-onto” approach. Using NaBH4 as a reducing agent, and DexPNI as a nucleating and stabilizing agent, the AuNPs can be obtained at ambient temperature within a short reaction time. Different features of AuNPs, such as their morphologies, optical properties and temperature-responsive behaviours are found to be dependent on the dosage of the gold precursor. The DexPNI-stabilized AuNPs not only show excellent stability against heat, high salt concentration and extreme pH, but could also be readily redispersed after freeze-drying. UV measurements and kinetic analysis of the AuNPs-catalyzed reduction of 4-nitrophenol at different temperatures illuminated that the optical properties and catalytic activity of AuNPs are closely related to temperature. Compared with previously reported diffusion-regulated nanoreacters, our AuNPs provide a unique opportunity to control the reaction rate in an inverse temperature-responsive manner at 32–35 °C, and further switch off the reaction at temperatures higher than 35 °C. These temperature-responsive properties could be used to create a smart sensor and catalyst, acting as an optical temperature alarm and recloser when the reaction temperature accidentally goes beyond the limit value. By using monomers and colloidal precursors other than NIPAAm and HAuCl4, it will be straightforward to extend the present route to build a variety of robust and smart nanomaterials with unprecedented properties.
Co-reporter:Xiaobin Fan, Guoliang Zhang and Fengbao Zhang
Chemical Society Reviews 2015 - vol. 44(Issue 10) pp:NaN3035-3035
Publication Date(Web):2015/03/17
DOI:10.1039/C5CS00094G
Scientific interest in graphene as a catalyst and as a catalyst support in heterogeneous catalytic reactions has grown dramatically over the past several years. The present critical review summarizes the multiple roles of graphene in heterogeneous catalysis and highlights the influence of defects, heteroatom-containing functionalities, and graphene's two-dimensional structure on catalytic performance. We first discuss the role and advantages of graphene as a catalyst support, with emphasis on its interactions with the catalytic phases and the influence of mass transfer processes. We then clarify the origin of the intrinsic catalytic activity of graphene in heterogeneous catalytic reactions. Finally we suggest challenges and potential practical applications for graphene in industrial processes.
Co-reporter:Qingshan Zhao, Yang Li, Ru Liu, Ao Chen, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2013 - vol. 1(Issue 47) pp:NaN15045-15045
Publication Date(Web):2013/10/03
DOI:10.1039/C3TA13378H
Graphene oxide (GO) is a promising support for anchoring homogeneous metal complexes because of its two-dimensional structure, huge surface area and diversity for chemical functionalizations. In this study, a ruthenium supported catalyst has been synthesized by covalently bonding a ruthenium complex (RuCl2(PPh3)3) onto the GO surface through coordination interaction with aminosilane ligand spacers. The supported catalyst showed enhanced catalytic performance towards hydrogenation of olefins and ketones compared with the homogeneous analogue, and it could be readily recycled and reused several times without discernible loss of its activity.
Co-reporter:Junyi Ji, Guanghui Zhang, Hongyu Chen, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2011 - vol. 21(Issue 38) pp:NaN14501-14501
Publication Date(Web):2011/08/11
DOI:10.1039/C1JM12970H
Graphene sheets decorated with metal/metal oxide nanoparticles are gaining increasing attention. In this study, sulfhydrylated graphene was prepared by reducing the sulfonic acid groups on sulfonated graphene to thiol groups. We evaluated its ability to anchor different metal/metal oxide nanoparticles by simply mixing the sulfhydrylated graphene with the corresponding pre-prepared metal/metal oxide nanoparticles. The sulfhydrylated graphene and its nanohybrids were characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), high-resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectroscopy (XPS). We demonstrate that the obtained sulfhydrylated graphene can act as a general platform to anchor different kinds of metal/metal oxide nanoparticles with different shapes, structures or properties through thiol–metal bonds. These novel hybrids will render graphene with additional interesting properties and potential applications.
Co-reporter:Jun Wang, Jingwen Ma, Xiaojie Li, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Chemical Communications 2014 - vol. 50(Issue 91) pp:NaN14240-14240
Publication Date(Web):2014/09/25
DOI:10.1039/C4CC06869F
Mesoporous Cu2O spheres with a large pore size (LP-Cu2O) bring out a better performance towards the photocatalytic aza-Henry reaction than Cu2O spheres with a small pore size (SP-Cu2O). This work highlights the internal diffusion coefficient as a critical parameter for the fabrication of porous photocatalysts.
Co-reporter:Yang Li, Hongyu Chen, Lian Yeau Voo, Junyi Ji, Guanghui Zhang, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2012 - vol. 22(Issue 30) pp:NaN15024-15024
Publication Date(Web):2012/05/28
DOI:10.1039/C2JM32307A
Partially hydrogenated graphene was readily prepared by an interesting reaction between graphene oxide and phenylboronic acid. This partially hydrogenated graphene was employed to synthesize brominated graphene through subsequent radical hydrogen abstraction.
Co-reporter:Yuanzhi Zhu, Man Qiao, Wenchao Peng, Yang Li, Guoliang Zhang, Fengbao Zhang, Yafei Li and Xiaobin Fan
Journal of Materials Chemistry A 2017 - vol. 5(Issue 19) pp:NaN9278-9278
Publication Date(Web):2017/03/31
DOI:10.1039/C7TA01438D
Metal-free carbon quantum dots (CQDs) have attracted great interest, but the rapid preparation of doped CQDs with tunable optical properties is still an urgent task. Herein, we report that covalent organic frameworks (covalent triazine-based frameworks, CTF-1) with layered structures can be rapidly exfoliated and cut into N-doped CQDs. The cutting mechanism involves triazine hydrolysis and breaking the bonds between the triazines and benzene rings. Experiments and density functional theory (DFT) calculations confirm that the fluorescence of the obtained CQDs mainly originates from the intrinsic state emission induced by localized π–π* transitions, despite the contribution of the defect state emission. Due to their unique chemical structure, the CQDs could be further utilized as an efficient PL probe for detecting Hg2+. This study may open up new avenues for developing new kinds of CQDs using covalent organic frameworks as the starting materials.
Co-reporter:Qingshan Zhao, Yuanzhi Zhu, Zhen Sun, Yang Li, Guoliang Zhang, Fengbao Zhang and Xiaobin Fan
Journal of Materials Chemistry A 2015 - vol. 3(Issue 6) pp:NaN2616-2616
Publication Date(Web):2014/12/02
DOI:10.1039/C4TA05205F
In this study, we develop a facile strategy to combine an organic amine with a palladium complex on graphene oxide (GO) as a cooperative catalyst for Tsuji–Trost allylation. A tertiary amine and palladium–diamine complex are simultaneously immobilized on a GO support through silylation and further in situ coordination processes. PdCl2 is employed as the palladium precursor, with no necessity for extra coordination ligands. Various characterizations confirm the successful preparation of the cooperative supported catalyst (GO–NEt2–2N–Pd). Systematic investigation reveals the immobilized palladium–diamine complex (GO–2N–Pd) with very low Pd loading is effective for Tsuji–Trost allylation, and incorporation of the tertiary amine shows a significant promoting effect towards the catalytic activity. GO–NEt2–2N–Pd can be readily recovered and recycled several times without reduction of its efficiency. Its excellent performance should be ascribed to synergistic catalysis effect, excellent support properties, and robust immobilization interaction.
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