Co-reporter:Cheng Chen, Li-Xuan Cai, Bin Tan, Ya-Jun Zhang, Xiao-Dong Yang, Shen Lin, and Jie Zhang
Crystal Growth & Design April 5, 2017 Volume 17(Issue 4) pp:1843-1843
Publication Date(Web):February 22, 2017
DOI:10.1021/acs.cgd.6b01809
A flexible bipyridinium ligand has been introduced into a series of isomorphous metal–organic frameworks to yield porous materials with subtriangular 1D channel and cagelike pore space. The introduction of bipyridinium molecules into the porous frameworks leads to the formation of 1D channel with positively charged surface, which shows high affinities to polar molecules such as methanol, ethanol, and water vapor. Additionally, the bipyridinium molecules possess conjugated pyridyl rings connected by carbon–carbon single bonds, which can rotate freely to keep twisted or large-conjugated planar configuration by controlling coordination condition during the self-assembly process. The cagelike pore space formed by these flexible bipyridinium molecules contains arene–arene stacked pyridyl rings and thus renders abundant π–π interaction sites for efficient adsorption of benzene and toluene molecules, and is also large enough to accommodate cyclohexane molecules. These metal–organic frameworks show efficient adsorption for benzene, toluene, and cyclohexane molecules through high utilization efficiency of unique pore space, and display rarely broad-spectrum adsorptivity to various organic pollutants with hydrophilic/hydrophobic, conjugated/nonconjugated characteristics.
Co-reporter:Shuhong Xu, Zhongshui Li, Fengling Lei, Yanli Wang, Yixin Xie, Shen Lin
Applied Surface Science 2017 Volume 426(Volume 426) pp:
Publication Date(Web):31 December 2017
DOI:10.1016/j.apsusc.2017.07.166
•PDDA and HCOOH were as structure-directing agent and reducing agent, respectively.•Core-shell hydrangea-like Pd@Pt nanocluster was obtained by step by step reduction.•Hydrangea-like Pd@Pt bimetal favors high exposure and good dispersion of Pt shell.•Pd@Pt nanocluster leads to stronger electronic coupling and less dissolution of Pd.•Pd@Pt/GNs (PDDA) exhibits an efficient catalytic performance for methanol oxidation.Core-shell palladium@platinum/graphene composite (denoted as Pd@Pt/GNs (PDDA)) was synthesized by successive reduction with formic acid as a reducing agent and poly(diallyldimethylammonium chloride) solution (PDDA) as a structure-directing agent at ambient temperature. The as-synthesized Pd@Pt/GNs (PDDA) was characterized by transmission electron microscopy (TEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The results indicate that hydrangea-like PtPd bimetallic nanoclusters on graphene (GNs) are formed with the aid of morphology control of PDDA. Especially, they are in a typical core-shell structure with Pd as core and Pt as shell, which are uniformly dispersed on the surface of GNs. Electrocatalytic tests show that Pd@Pt/GNs (PDDA) exhibits superior electrocatalytic activity for methanol oxidation (with the mass activities of 870.8 mA mg−1 Pt) in comparison with the commercial Pt/C and alloyed Pd-Pt/GNs (PDDA) catalysts owing to its unique Pd core Pt shell hydrangea-like structure and the synergistic effects between Pd@Pt and GNs.Download high-res image (161KB)Download full-size image
Co-reporter:Qiuling Wu;Meiling Jiang;Xiaofeng Zhang;Jiannan Cai
Journal of Materials Science 2017 Volume 52( Issue 11) pp:6656-6669
Publication Date(Web):16 February 2017
DOI:10.1007/s10853-017-0901-4
Octahedral MnO/reduced graphene oxide (RGO) composite was synthesized by thermal decomposition method and characterized by XRD, Raman, XPS, TGA/DSC, TEM and SEM. The analysis results show that GO was reduced to RGO, and the octahedral MnO nanoparticles disperse on the RGO sheet by thermal decomposition process. It is important that the as-prepared composite exhibits excellent electrocatalytic performance for oxygen reduction reaction. The onset potential of the octahedral MnO/RGO composite is about 100 and 200 mV positive-shifted compared with that of MnO and RGO, respectively. The current density of O2 reduction for the MnO/RGO composite is also much higher than that of MnO and RGO, respectively. In addition, the composite shows better stability and tolerance ability toward CH3OH and CO poisoning than that of commercial Pt-based catalyst. The enhanced electrocatalytic performance of octahedral MnO/RGO may make it available to be an efficient and cheap noble-metal free cathodic catalyst for fuel cells and metal–air batteries.
Co-reporter:Zhongshui Li, Lingting Ye, Fengling Lei, Yanli Wang, Shuhong Xu, Shen Lin
Electrochimica Acta 2016 Volume 188() pp:450-460
Publication Date(Web):10 January 2016
DOI:10.1016/j.electacta.2015.11.149
•Pt (Pd)/ZnO/GNs composite was synthesized via one-pot hydrothermal process.•Highly dispersed Pt (Pd) nanoparticles are assembled onto Pt (Pd)/ZnO/GNs composite.•Pt (Pd)/ZnO/GNs serves as an efficient electro-photo synergistic catalyst for MOR.•Electro-photo synergistic catalysis is realized under UV/visible light irradiation.•ZnO bandgap narrowing favors better synergistic effect in visible light irradiation.One-pot method is used to synthesize Pt (Pd)/ZnO/graphene composite (simplified as Pt (Pd)/ZnO/GNs). Under hydrothermal conditions, weak basic Zn2+ ions (pH = 9.0) is converted to ZnO, accompanying synchronous reduction of K2PtCl4 (K2PdCl4) and graphene oxide (GO) without additional reducing agent. ZnO deposited on the surface of graphene nanosheets (GNs) offers homogeneous nuclei to anchor metal particles, leading to the uniform dispersion of Pt (Pd) particles, with average diameter of 3.0 nm for Pt and 5.5 nm for Pd. Electrochemical experiments show that Pt/ZnO/GNs and Pd/ZnO/GNs have much higher catalytic activity and stability for methanol oxidation reaction (MOR) and improved tolerance of CO compared with commercially available Johnson Matthey 20% Pt/C catalyst (Pt/C-JM) and Sigma-Aldrich 20% Pd/C catalyst (Pd/C-SA). Under light irradiation, catalytic activities of Pt (Pd)/ZnO/GNs are drastically enhanced, with the mass activities of 1724.2 mA mg−1 (UV irradiation) & 1935.5 mA mg−1 (visible irradiation) for Pt/ZnO/GNs, and 733.5 mA mg−1 (UV irradiation) & 818.3 mA mg−1 (visible irradiation) for Pd/ZnO/GNs. The improved performance mainly derives from the synergistic effects between the electro-catalysis of well dispersed Pt (Pd) nanoparticles and photo-catalysis of ZnO. And the band gap narrowing of ZnO in Pt (Pd)/ZnO/GNs contributes to the enhanced synergistic catalysis effects under visible light irradiation, which provides new opportunities for exploiting efficient visible light assisted electro-catalytic methanol oxidation reaction.
Co-reporter:Fengling Lei, Zhongshui Li, Lingting Ye, Yanli Wang, Shen Lin
International Journal of Hydrogen Energy 2016 Volume 41(Issue 1) pp:255-264
Publication Date(Web):5 January 2016
DOI:10.1016/j.ijhydene.2015.09.098
•Pt/SnO2/GNs (EDTA) composite was synthesized by one-pot hydrothermal process.•EDTA makes size optimization of Pt and homogeneous coexistence of SnO2 and Pt.•Pt/SnO2/GNs (EDTA) show superior catalytic activity for MOR under light irradiation.•The introduction of SnO2 brings about electro-photo catalysis under light irradiation.•Electro-photo synergistic catalysis contributes to superior catalytic performance.In this work, a simple one-pot strategy was used to synthesize an anodic electrocatalyst Pt/SnO2/GNs (EDTA) for direct methanol fuel cells (DMFCs). Under hydrothermal conditions, the reduction of H2PtCl6 and graphene oxide (GO), the oxidation of SnCl2 and the formation of SnO2 were occurred synchronously without additional reducing or oxidizing agent. The introduction of EDTA results in good dispersion and full integration of Pt and SnO2 nanoparticles, due to the complexation between Pt4+ (Sn2+) and EDTA. Electrochemical experiments show Pt/SnO2/GNs (EDTA) has much higher catalytic activity and better stability for MOR compared with the commercial Pt/C catalyst and Pt/GNs (EDTA). Furthermore, it is interesting to find that catalytic properties of Pt/SnO2/GNs (EDTA) toward MOR are significantly enhanced under external light irradiation. Especially, after UV irradiation for 30 min, Pt/SnO2/GNs (EDTA) composite shows an ultrahigh forward peak current density of 1103 mA mg−1. The remarkably improved performances under external light irradiation mainly derives from the synergistic effects between the electro-catalytic and photo-catalytic properties, which provides a novel strategy to effectively enhance the catalytic activities of Pt catalyst in DMFCs by coupling with photoresponsive metal oxides.
Co-reporter:Zhongshui Li, Lingting Ye, Yanli Wang, Shuhong Xu, Fengling Lei and Shen Lin
RSC Advances 2016 vol. 6(Issue 83) pp:79533-79541
Publication Date(Web):16 Aug 2016
DOI:10.1039/C6RA17309H
In this work, a facile method was used to synthesize the heterostructured bimetallic catalyst Pd–Ag/graphene (simplified as Pd–Ag/GNs). In order to achieve the heterostructured Pd–Ag nanoparticles (NPs), Ag2O was firstly produced on GNs from AgOH under UV irradiation, then the heterogeneous phase between the precursor Pd2+ and Ag2O contributes to the formation of the highly dispersed heterostructured Pd–Ag NPs with the average diameter of 5 nm on GNs after a synchronous reduction process. Electro-catalytic performances of Pd–Ag/GNs were investigated by cyclic voltammetry (CV), chronoamperometry, COad stripping voltammetry, and electrochemical impedance spectroscopy (EIS). It is shown that Pd–Ag/GNs has a much higher catalytic activity (595 mA mg−1) and stability for methanol oxidation reaction (MOR) and improved tolerance of CO compared with the counterpart Pd/GNs and the commercial 20% Pd/C catalyst (Pd/C-SA). And under visible light irradiation, the catalytic activity and stability of Pd–Ag/GNs are remarkably enhanced. Especially, its mass activity is 1128 mA mg−1 which is 1.9 times higher than that without light irradiation. The significantly improved performance benefits from the efficient electro–photo synergistic catalysis for MOR under visible light irradiation, which is in favor of harvesting sunlight to produce clean energy.
Co-reporter:Qiufeng HuangQingshuai Han, Shurong Fu, Zizhu Yao, Lv Su, Xiaofeng Zhang, Shen Lin, Shengchang Xiang
The Journal of Organic Chemistry 2016 Volume 81(Issue 24) pp:12135-12142
Publication Date(Web):November 14, 2016
DOI:10.1021/acs.joc.6b01200
An efficient synthesis of 6H-isoindolo[2,1-a]indol-6-ones through rhodium-catalyzed NH-indole-directed C–H carbonylation of 2-arylindoles with carbon monoxide has been developed. Preliminary mechanistic studies revealed that this reaction proceeds via N–H bond cleavage and subsequent C–H bond cleavage. Reaction monitoring via ESI-MS was used to support the formation of five-membered rhodacycle species in the catalytic cycle.
Co-reporter:Xiaofeng Zhang, Xiaoying Wang, Lijuan Le, Ai Ma and Shen Lin
Journal of Materials Chemistry A 2015 vol. 3(Issue 38) pp:19273-19276
Publication Date(Web):20 Aug 2015
DOI:10.1039/C5TA04450B
Octahedral Fe3O4 crystals were prepared by a facile potentiostatic deposition approach. The as-prepared Fe3O4 exhibits high electrocatalytic activity toward the oxygen reduction reaction (ORR) and excellent stability. The unique octahedral structure provides a high density of active sites and facilitates the ORR via a dominant pathway of oxygen reduction to hydroxide.
Co-reporter:Ai Ma, Xiaofeng Zhang, Xiaoying Wang, Lijuan Le and Shen Lin
RSC Advances 2015 vol. 5(Issue 79) pp:64534-64537
Publication Date(Web):23 Jul 2015
DOI:10.1039/C5RA09492E
PdCu alloy nanoparticles (with sizes of ca. 4.5 nm) have been synthesized by a one-step electrochemical process on composite films constructed from functionalized graphene (GN) and H3PMo12O40 (PMo12) by LBL assembly. The as-prepared hybrid displays enhanced eletrocatalytic activity and extended durability towards formic acid oxidation in an acid media.
Co-reporter:Xiu-Hong Yang;Ming-Xing Yang;Li-Juan Chen;Jing Guo
Acta Crystallographica Section C 2015 Volume 71( Issue 5) pp:369-373
Publication Date(Web):
DOI:10.1107/S2053229615005823
The title compound, [Cd3(C8H10O4)3(C12H9N3)2(H2O)2]n or [Cd3(chdc)3(4-PyBIm)2(H2O)2]n, was synthesized hydrothermally from the reaction of Cd(CH3COO)2·2H2O with 2-(pyridin-4-yl)-1H-benzimidazole (4-PyBIm) and cyclohexane-1,4-dicarboxylic acid (1,4-chdcH2). The asymmetric unit consists of one and a half CdII cations, one 4-PyBIm ligand, one and a half 1,4-chdc2− ligands and one coordinated water molecule. The central CdII cation, located on an inversion centre, is coordinated by six carboxylate O atoms from six 1,4-chdc2− ligands to complete an elongated octahedral coordination geometry. The two terminal rotationally symmetric CdII cations each exhibits a distorted pentagonal–bipyramidal geometry, coordinated by one N atom from 4-PyBIm, five O atoms from three 1,4-chdc2− ligands and one O atom from an aqua ligand. The 1,4-chdc2− ligands possess two conformations, i.e.e,e-trans-chdc2− and e,a-cis-chdc2−. The cis-1,4-chdc2− ligands bridge the CdII cations to form a trinuclear {Cd3}-based chain along the b axis, while the trans-1,4-chdc2− ligands further link adjacent one-dimensional chains to construct an interesting two-dimensional network.
Co-reporter:Ming-Xing Yang, Shen Lin, Li-Juan Chen, Xiao-Hua Chen, Xiu-Hong Yang, Jing Guo
Polyhedron 2015 Volume 87() pp:329-337
Publication Date(Web):17 February 2015
DOI:10.1016/j.poly.2014.11.021
Three new polyoxometalate-based metal–organic framework compounds [Ag7(3-pttz)4(PMo12O40)]·H2O(1), [Ag6(3-Hpttz)2(3-pttz)2(SiMo12O40)(H2O)2]·2H2O(2) and [Ag6(3-Hpttz)6(PMo12O40)2]·2H2O(3) (3-Hpttz = 5-(3-Pyridyl)-1H-tetrazole) are synthesized hydrothermally by changing the polyoxoanions and the pH values in the same metal–organic system (Ag/pttz), and structurally characterized by IR spectra, elemental analyses and single crystal X-ray diffraction. Compound 1 exhibits a three-dimensional (3D) Ag/3-pttz host framework with larger channels. The discrete [PMo12O40]3− anions, acting as inorganic templates, are embedded in the channels. In compound 2, the Ag/3-pttz motif displays a two-dimensional (2D) stair-like layer, which is linked by [SiMo12O40]4− anions to construct a 3D framework. In compound 3, the Ag/3-pttz motif shows a 1D ribbon-like chain, some of [PMo12O40]3− anions in a “shoulder-to-shoulder” mode link two ribbon-like polymers to form a 1D “quadrangular prism-like” chains, and the others of [PMo12O40]3− anions bond to chains and become pendants of the quadrangular prism, projecting toward two sides. Therefore, compound 3 displays a scarce 1D “quadrangular prism with pendants” structure. In addition, the electrochemical behavior and electrocatalytic activity of compound 1 as an example were investigated.Three POM-based MOFs containing 1D to 3D Ag/3-pttz coordination polymers were successfully synthesized by changing kinds of inorganic salt which containing the center element of the Keggin heteropolymolybdate and pH values.
Co-reporter:Zhongshui Li;Fengling Lei;Lingting Ye;Xiaofeng Zhang
Journal of Nanoparticle Research 2015 Volume 17( Issue 4) pp:
Publication Date(Web):2015 April
DOI:10.1007/s11051-015-2995-4
Controlled assembly in aqueous solution was used to synthesize the well-organized Pt/CS/PW12-GNs composite. By the aid of linear cationic polysaccharide chitosan, 2-D distribution worm-like Pt nanoparticles with their length and width of 15–20 and 3–4 nm, respectively, were formed on the surface of CS/PW12-GNs using HCOOH as a reducing agent at room temperature. The introduction of CS leads to well dispersion of worm-like Pt nanoparticles, the electroactivity of H3PW12O40 (PW12) alleviates CO poisoning toward Pt particles, and graphene nanosheets (GNs) ensure excellent electrical conductivity of the composites. The combined action among different components results in significantly enhanced catalytic activity of Pt/CS/PW12-GNs toward methanol oxidation and better tolerance of CO. The as-synthesized Pt/CS/PW12-GNs exhibit the forward peak current density of 445 mA mg−1, which is much higher than that (220 mA mg−1) for Pt/C-JM (the commercially available Johnson Matthey Hispec4000 catalyst, simplified as Pt/C-JM) and some recently reported Pt/graphene-based nanomaterials. The construction of 2-D distribution worm-like Pt nanoparticles and facile wet chemical synthesis strategy provide a promising way to develop superior performance electrocatalysts for direct methanol fuel cells applications.
Co-reporter:Lingting Ye, Zhongshui Li, Xiaofeng Zhang, Fengling Lei and Shen Lin
Journal of Materials Chemistry A 2014 vol. 2(Issue 48) pp:21010-21019
Publication Date(Web):13 Oct 2014
DOI:10.1039/C4TA05094K
A facile one-pot method was used to synthesize Pt/Cu2O/GNs and Pd/Cu2O/GNs composites. Pt or Pd nanoparticles are deposited onto graphene sheets (GNs) and Cu2O via synchronous reduction of K2PtCl4 (K2PdCl4), Cu(OH)2 and graphene oxide (GO) with glucose as a reducing agent under microwave irradiation. The formation of Cu2O promotes the nucleation of Pt(0) or Pd(0) particles and favors more complete reduction of PtCl42− or PdCl42−. Catalytic properties of as-prepared composites for methanol oxidation reaction (MOR) were evaluated by cyclic voltammetry (CV), chronoamperometry, COads stripping voltammetry and electrochemical impedance spectrum (EIS). Electrochemical experiments showed that Pt/Cu2O/GNs and Pd/Cu2O/GNs had much higher catalytic activity and stability for MOR and better resistance to CO poisoning compared with the commercially available Johnson Matthey 20% Pt/C catalyst (Pt/C-JM) and Sigma-Aldrich 20% Pd/C catalyst (Pd/C-SA). Especially under the UV irradiation, the total peak current density and catalytic stability of Pt/Cu2O/GNs and Pd/Cu2O/GNs drastically increase, which may result from the synergistic effect between the electro-catalytic and photo-catalytic properties. In brief, the cooperation among Pt (Pd), Cu2O and GNs promotes remarkably the catalytic performance for MOR on Pt/Cu2O/GNs and Pd/Cu2O/GNs either without light or with UV irradiation.
Co-reporter:Zhongshui Li, Lian Zhang, Xiaomei Huang, Lingting Ye, Shen Lin
Electrochimica Acta 2014 Volume 121() pp:215-222
Publication Date(Web):1 March 2014
DOI:10.1016/j.electacta.2013.12.174
•Graphene nanosheets and β-cyclodextrin were integrated by a facile chemical procedure.•GNs-CD was used as a support to load nanodendritic hydrangea-like Pt nanoclusters.•hydrophobic interaction between CD and Pt particle regulated nanocluster morphology.•GNs functioned as a matrix to distribute Pt nanoclusters uniformly.•Pt/GNs-CD showed remarkably enhanced catalytic activities for methanol oxidation.The integration of graphene nanosheets (GNs) and β-cyclodextrin (CD) may bring about large surface area and high conductivity of GNs and unique supramolecular recognition capability of CD together. In this paper, for the first time, GNs-CD was used as a supporting material to construct nanodendritic hydrangea-like Pt nanoparticles, which was implemented by a facile wet chemical procedure. β-CD on GNs surface was used to regulate the final morphology of Pt nanoparticles without additional capping agent and seeds, and GNs functioned as a matrix to obtain a relatively uniform distribution of Pt nano-clusters. Electrocatalytic performance of the as-prepared Pt/GNs-CD hybrid was investigated by cyclic voltammetry (CV), chronoamperometry, COad stripping voltammetry, and electrochemical impedance spectroscopy (EIS). The Pt/GNs-CD hybrid exhibited much higher catalytic activity and stability than Pt/GNs and Pt/Vulcan X72R towards methanol oxidation, suggesting that Pt/GNs-CD hybrid could be a promising electrocatalyst for high-performance direct methanol fuel cells (DMFCs) applications.
Co-reporter:Lingting Ye, Zhongshui Li, Lian Zhang, Fengling Lei, Shen Lin
Journal of Colloid and Interface Science 2014 Volume 433() pp:156-162
Publication Date(Web):1 November 2014
DOI:10.1016/j.jcis.2014.06.012
•Pt/TiO2/GNs were synthesized using ethanol as reductant under microwave irradiation.•TiO2 accelerated reduction reaction and promoted heterogeneous nucleation of Pt.•Unique Pt nanoclusters were formed around TiO2 supported on GNs.•Composites show an ultrahigh catalytic activity for MOR under UV irradiation.•Electro-photo-synergistic effect is responsible for remarkably improved catalysis.A facile and green one-pot method was used to synthesize Pt/TiO2/Graphene composites with ethanol as a reducing agent under microwave irradiation. The as-prepared composites were characterized by SEM, TEM, EDX, XPS, XRD and Raman. Electrocatalytic performance of the Pt/TiO2/GNs composites was investigated by cyclic voltammetry (CV), chronoamperometric (CA), COad stripping voltammetry and electrochemical impedance spectrum (EIS). All experimental data have revealed that TiO2 (P25) not only enhanced the reduction ability of ethanol under microwave irradiation but also promoted Pt heterogeneous nucleation to form Pt nanoclusters which are around P25 and loaded on graphene nanosheets (GNs) surface. Electrochemical experiments showed that Pt/TiO2/GNs had much higher catalytic activity and stability toward methanol oxidation reaction (MOR) and better resistance to CO poisoning compared with Pt/GNs and the commercially available Johnson Matthey 20% Pt/C catalyst (Pt/C-JM). Especially under UV irradiation with 20 min, Pt/TiO2/GNs composites showed an ultrahigh forward peak current density of 1354 mA mg−1, nearly 2.5 times higher than that of Pt/C-JM, which indicated that the electrocatalytic and photocatalytic properties of Pt/TiO2/GNs had been integrated to boost the catalytic performance for MOR.
Co-reporter:Xiao-Hua Chen;Hua Huang;Ming-Xing Yang;Li-Juan Chen
Acta Crystallographica Section C 2014 Volume 70( Issue 5) pp:488-492
Publication Date(Web):
DOI:10.1107/S2053229614007992
In poly[aqua(μ3-benzene-1,4-dicarboxylato-κ5O1,O1′:O1:O4,O4′)[2-(pyridin-3-yl-κN)-1H-benzimidazole]cadmium(II)], [Cd(C8H4O4)(C12H9N3)(H2O)]n, (I), each CdII ion is seven-coordinated by the pyridine N atom from a 2-(pyridin-3-yl)benzimidazole (3-PyBIm) ligand, five O atoms from three benzene-1,4-dicarboxylate (1,4-bdc) ligands and one O atom from a coordinated water molecule. The complex forms an extended two-dimensional carboxylate layer structure, which is further extended into a three-dimensional network by hydrogen-bonding interactions. In catena-poly[[diaquabis[2-(pyridin-3-yl-κN)-1H-benzimidazole]cobalt(II)]-μ2-benzene-1,4-dicarboxylato-κ2O1:O4], [Co(C8H4O4)(C12H9N3)2(H2O)2]n, (II), each CoII ion is six-coordinated by two pyridine N atoms from two 3-PyBIm ligands, two O atoms from two 1,4-bdc ligands and two O atoms from two coordinated water molecules. The complex forms a one-dimensional chain-like coordination polymer and is further assembled by hydrogen-bonding interactions to form a three-dimensional network.
Co-reporter:Qing-Biao Hou;Li-Juan Chen;Jing Guo
Acta Crystallographica Section C 2014 Volume 70( Issue 3) pp:302-305
Publication Date(Web):
DOI:10.1107/S2053229614003696
A novel neutral polymer, {[Co2(C7H3NO4)2(H2O)4]·2H2O}n, was hydrothermally synthesized using pyridine-2,5-dicarboxylate (2,5-PDC2−) as the organic linker. It features a two-dimensional layer structure constructed from one-dimensional {[Co(2,5-PDC)2]2−}n chains interlinked by [Co(H2O)4]+ units. The two CoII cations occupy special positions, sitting on inversion centres. Each 2,5-PDC2− anion chelates to one CoII cation via the pyridine N atom and an O atom of the adjacent carboxylate group, and links to two other CoII cations in a bridging mode via the O atoms of the other carboxylate group. In this way, the 2,5-PDC2− ligand connects three neighbouring CoII centres to form a two-dimensional network. The two-dimensional undulating layers are linked by extensive hydrogen bonds to form a three-dimensional supramolecular structure, with the uncoordinated solvent molecules occupying the interlamellar region.
Co-reporter:Xiaofeng Zhang, Qiufeng Huang, Zhongshui Li, Ai Ma, Xiaolei He, Shen Lin
Materials Research Bulletin 2014 60() pp: 57-63
Publication Date(Web):
DOI:10.1016/j.materresbull.2014.08.014
Co-reporter:Dr. Qiufeng Huang;Shaojia Ke;Lin Qiu;Xiaofeng Zhang;Dr. Shen Lin
ChemCatChem 2014 Volume 6( Issue 6) pp:
Publication Date(Web):
DOI:10.1002/cctc.201490035
Co-reporter:Dr. Qiufeng Huang;Shaojia Ke;Lin Qiu;Xiaofeng Zhang;Dr. Shen Lin
ChemCatChem 2014 Volume 6( Issue 6) pp:1531-1534
Publication Date(Web):
DOI:10.1002/cctc.201400091
Abstract
An efficient and selective C2 alkenylation of benzofurans was performed by using Pd(OAc)2 combined with a catalytic amount of 11-molybdovanadophosphoric acid (H4PMo11VO40) under an atmosphere of dioxygen. N-Acetylglycine (Ac-Gly-OH) was observed to be an effective additive for the olefination reaction.
Co-reporter:Qiufeng Huang;Qianqian Song;Jin Cai;Xiaofeng Zhang
Advanced Synthesis & Catalysis 2013 Volume 355( Issue 8) pp:1512-1516
Publication Date(Web):
DOI:10.1002/adsc.201201114
Abstract
An efficient and practical synthetic method has been developed for the preparation of 3-vinylindoles by the direct CH olefination of indoles with alkenes. The transformation is catalyzed by palladium acetate combined with 12-molybdophosphoric acid and uses oxygen as the terminal oxidant. 4-Dimethylaminopyridine (DMAP) was observed to be an effective additive for the olefination reaction. Functional groups such as methoxy, benzyloxy, fluoro, bromo, ester, phenyl, and methyl were tolerated under the reaction conditions.
Co-reporter:Xiaofeng Zhang, Qiufeng Huang, Bingtai Ke, Xiaoling Huang, XuePing Chen, Shen Lin
Journal of Luminescence 2013 Volume 138() pp:117-121
Publication Date(Web):June 2013
DOI:10.1016/j.jlumin.2013.01.022
Multilayer films consisting of poly(amidoamine) (PAMAM) dendrimer and europium-substituted heteropolymolybdate K17[Eu(P2Mo17O61)2] (simplified as Eu(P2Mo17)2) were prepared by layer-by-layer (LBL) self-assembly and characterized by UV–vis measurements, X-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM). UV–vis showed that the characteristic absorbance values of the multilayer films increased linearly with the layer numbers of Eu(P2Mo17)2/PAMAM films. The electrostatic interaction between Eu(P2Mo17)2 and PAMAM was demonstrated by XPS. In addition, AFM provided the surface morphology of Eu(P2Mo17)2/PAMAM films, revealing that the films contained well-defined Eu(P2Mo17)2 nanoparticles. The luminescence behavior of the films at room temperature was also investigated. The films exhibited the characteristic emission bands of Eu3+ and the fluorescence lifetime of Eu3+ in the films is shorter than that in the solid.Highlights► Films based on Eu(P2Mo17)2 and PAMAM dendrimer have been prepared by LBL method. ► The films grow regularly and well-defined Eu(P2Mo17)2 nanoparticles can be achieved. ► The films exhibit the characteristic emission bands of the Eu3+ ion. ► Life time of Eu3+ is shorter in the films than in the solid.
Co-reporter:Kaicong Cai, Diwen Liu, Chenyu Lou, Shen Lin
Vibrational Spectroscopy 2013 Volume 66() pp:8-13
Publication Date(Web):May 2013
DOI:10.1016/j.vibspec.2013.01.005
In the present study, anharmonic vibrational properties of the amide modes in N-methylacetamide (NMA), a model molecule for peptide vibrational spectroscopy, are examined by DFT calculations. The 3N-6 normal mode frequencies, diagonal and off-diagonal anharmonicities are evaluated by means of the second order vibrational perturbation theory (VPT2). Good performance of B3LYP/6-31+G** is found for predicting vibrational frequencies in comparison with gas phase experimental data. The amide vibrational modes are assigned through potential energy distribution analysis (PED). The solvation effect on the amide vibrational modes is modeled within the PCM method. From gas phase to polar solvents, red shifts are observed for both harmonic and anharmonic vibrational frequency of amide I mode while the CO bond length increases upon the solvent polarity. Cubic and quartic force constants are further calculated to evaluate the origin of the anharmonicity for the amide I mode of NMA in different micro-environments.
Co-reporter:Xiaoju Li, Xiaofang Guo, Xiahong Xu, Guangchao Ma, Shen Lin
Inorganic Chemistry Communications 2013 Volume 27() pp:105-107
Publication Date(Web):January 2013
DOI:10.1016/j.inoche.2012.10.031
An eight-connected 3D coordination polymer consisting of water-bridged dinuclear Ni(II) units has been prepared. The complex exhibits an unprecedented non-interpenetrating framework.An eight-connected 3D coordination polymer has been synthesized and characterized. The complex is non-interpenetrating and consists of the water-bridged dinuclear Ni(II) units.Highlights► A 3D coordination polymer consisting of dinuclear Ni(II) units was prepared. ► The complex is an eight-connected network. ► The framework of the complex is non-interpenetrating.
Co-reporter:Zhongshui Li, Xiaomei Huang, Xiaofeng Zhang, Lian Zhang and Shen Lin
Journal of Materials Chemistry A 2012 vol. 22(Issue 44) pp:23602-23607
Publication Date(Web):24 Sep 2012
DOI:10.1039/C2JM35239G
The {PEI-GNs/PMo12}n composite films are prepared by an LBL electrostatic assembly technique, and their uniform and homogeneous traits have been verified by UV-vis and cyclic voltammetry. The {PEI-GNs/PMo12}n composite films are used as a novel catalyst support for electro-deposition of Pt particles in situ. Pt particles immobilizing on the surface of {PEI-GNs/PMo12}n composite films were confirmed by XPS, EDX, XRD and FE-SEM. The interesting seashell-like Pt micro–nano-clusters can be obtained when {2PEI-GNs/PMo12} composite films are used as catalyst supports. Pt-{PEI-GNs/PMo12}n composite films present good electrocatalytic activity regarding methanol oxidation and improved tolerance of CO. These results indicate that poly(ethyleneimine) functionalized graphene (PEI-GNs) preserves the superior electric conductivities of graphene sheets in the composite films, and the introduction of electroactive [PMo12O40]3− (PMo12) into the composite films helps to convert intermediate species CO into CO2 from the Pt nanoparticles. The synergistic effect of PEI-GNs and PMo12 remarkably enhanced the electrocatalytic activity and stability regarding methanol oxidation.
Co-reporter:Xiaoju Li, Xiaofang Guo, XiuLan Weng and Shen Lin
CrystEngComm 2012 vol. 14(Issue 4) pp:1412-1418
Publication Date(Web):08 Dec 2011
DOI:10.1039/C1CE06216F
The reaction of 1,4-bis((pyridinium-4-carboxylic acid)methyl)benzene dibromide (Bpmb-2HBr), Cd(NO3)2·4H2O with 1,2-bis(imidazol-1′-yl)ethane (Bime) and 1,4-bis(imidazol-1′-yl)butane (Bimb) gave rise to two novel 2D Cd(II) coordination polymers, [Cd1.5(Bime)(Bpmb)0.5(μ-Br)Br2·DMF]n (1) and [Cd2(Bimb)2(μ-Br)2Br2]n (2), respectively, in which coordination of μ-Br− and monodentate Br− with Cd(II) generates an unprecedented trimeric [Cd3(μ-Br)2Br4] unit in 1 and a dimeric [Cd2(μ-Br)2Br2] unit in 2. In 1, gauche-Bime links the central six-coordinated Cd(II) of the trimers into a 1D double chain, anti-Bpmb further bridges the terminal four-coordinated Cd(II) of the trimers in the opposite direction to generate a 2D layer. Complex 2 is a 2D corrugated layer consisting of perpendicular left- and right-handed helical chains constructed through anti-anti-gauche-conformated Bimb bridging the neighboring six-coordinated Cd(II) of [Cd2(μ-Br)2Br2] units. The thermal stability and fluorescent properties of the two complexes have also been studied.
Co-reporter:Xiaofang Guo, Xiaoju Li, Xiulan Weng, Shen Lin
Journal of Molecular Structure 2012 Volume 1008() pp:63-68
Publication Date(Web):25 January 2012
DOI:10.1016/j.molstruc.2011.11.025
The reaction of 1,2-bis(imidazol-1′-yl)ethane (bime), 4-hydroxybenzoic acid (HO-HBC) with different metal salts in water/ethanol gave rise to three supramolecular architectures [M(HO-BC)2(H2O)2(bime)]n [M = Mn(II), Co(II) and Ni(II)]. Single crystal X-ray diffraction analysis reveals that complexes 1–3 are isomorphous and are 3D supramolecular networks. HO-BC serves as a monodentate ligand through one carboxylate oxygen atom coordinating to metal center. The extensive hydrogen bonds from HO-BC and coordination water result in the formation of 3D supramolecular networks. The gauche-conformational bime connects the neighboring metal ions into 1D chain, which is located in the large void of the 3D networks. The thermogravimetric analysis reveals that complexes 1–3 are stable before 273 °C. Magnetic analysis shows that there are no interactions between neighboring metal ions.
Co-reporter:Li-Juan Chen, Jiang-Bo Su, Rong-Bin Huang, Shen Lin, Ming-Xing Yang and Hua Huang
Dalton Transactions 2011 vol. 40(Issue 38) pp:9731-9736
Publication Date(Web):22 Aug 2011
DOI:10.1039/C1DT10723B
A 2D tri-layer compound {[Co8(tbip)6(H2O)9(OH)4]·12(H2O)}n (1) (H2tbip = 5-tert-butyl isophthalic acid) consisting of novel heptacobaltate clusters and single cobalt centers bridged by tbip2− ligands has been hydrothermally synthesized. The complex represents a rare example of a homometallic coordination polymer built up from both heptanuclear metal clusters and single metal centers simultaneously. The magnetic investigation reveals that the complex exhibits the overall predominance of antiferromagnetic coupling between magnetic centers.
Co-reporter:Xiaoju Li, Yuanzhu Cai, Zhenlan Fang, Lijian Wu, Bin Wei, and Shen Lin
Crystal Growth & Design 2011 Volume 11(Issue 10) pp:4517-4524
Publication Date(Web):September 2, 2011
DOI:10.1021/cg200730k
Three two-folded interpenetrating 3D coordination polymers, [M(ip-OH)(Bimb)0.5]n [where M = Ni(II) (1), Co(II) (2), or Cu(II) (3); H2ip-OH = 5-hydroxylisophthalic acid; and Bimb =1,4-bis(imidazol-1′-yl)butane], were synthesized by hydrothermal reactions of H2ip-OH, Bimb, and MCl2 in the presence of base. Single-crystal X-ray diffraction studies reveal that 1–3 consist of dinuclear metal units, which are bridged by ip-OH to form [M(ip-OH)]n layers and are further pillared by Bimb to generate 3D α-Po networks. Bimb adopts a gauche–antigauche conformation. Both the large void in the 3D network and the hydrogen bonds between hydroxyl of ip-OH and one carboxylate oxygen atom from the other network result in the formation of two-folded interpenetrating architectures. The secondary building units in 1–3 are well separated by ip-OH and Bimb. The magnetic data of 1–3 were fitted to the dimeric modes; fitting results indicate antiferromagnetic exchange between metal centers in the dinuclear metal units.
Co-reporter:Ming-Xing Yang, Li-Juan Chen, Shen Lin, Xiao-Hua Chen and Hua Huang
Dalton Transactions 2011 vol. 40(Issue 9) pp:1866-1872
Publication Date(Web):30 Nov 2010
DOI:10.1039/C0DT00781A
Three inorganic–organic compounds based on [MoxOy]n− chains, [Ag4(3-pttz)2Mo3O10] (1) (3-pttz = 5-(3-pyridyl) tetrazolate), [Ag4(2-pttz)2Mo4O13] (2) (2-pttz = 5-(2-pyridyl) tetrazolate), and [Ag4(pzttz)2Mo4O13] (3) (pzttz = 5-(pyrazinyl) tetrazolate), have been self-assembled, accompanied by in situ formation processes of the 5-substituted tetrazolate ligands under hydrothermal condition. Compound 1 features a 3D framework composed of [Mo3O10]2− chains cross-linked by [Ag4(3-pttz)2]2+ belts. Compounds 2 and 3 reveal the 3D structures based on [Mo4O13]2− chains pillared by silver tetrazolate polymeric chains. The three title compounds represent the first three examples that the tetrazolate ligands are introduced into the backbones of the [MoxOy]n− anion chains.
Co-reporter:Ming-Xing Yang, Shen Lin, Li-Juan Chen, Xiao-Feng Zhang, Hua Huang
Inorganic Chemistry Communications 2011 Volume 14(Issue 10) pp:1652-1655
Publication Date(Web):October 2011
DOI:10.1016/j.inoche.2011.06.031
Two hybrid compounds based on {Mo5O16} ribbon-like chains, [M(3-pt)2(Mo5O16)]·H2O (M = Co, Mn) (1 and 2) {3-pt = 5-(3-pyridyl)-tetrazole}, have been hydrothermally synthesized and characterized by single crystal X-ray diffraction. Three-dimensional Mo/O/MII/tetrazole frameworks of the title compounds are constructed from 1D infinite ribbon-like [Mo5O16]2− chains covalently linked through [M(3-ptz)]2+ fragments via OM and NMo coordinate bonds. It is noteworthy that the isostructural compounds contain an unprecedented 3D bimetallic oxide network with 16-membered wheel clusters in which two parallel interdigitated stacks of 3-pt ligands are trapped. Remarkably, the title complexes represent the first two examples of the solid materials containing {Mo5O16} ribbon-like chains.Two 3D Mo/O/MII/tetrazole framework compounds are constructed from 1D infinite ribbon-like [Mo5O16]2− chains covalently linked through [M(3-ptz)]2+ fragments via OM and NMo coordinate bonds. The title isostructural compounds contain an unprecedented 3D bimetallic oxide network with 16-membered wheel clusters in which two parallel interdigitated stacks of 3-pt ligands are trapped and represent the first two examples of the solid materials containing {Mo5O16} ribbon-like chains.Highlights► Two compounds show very interesting 3D bimetallic oxide networks. ► The 3D frameworks contain 16-membered wheel clusters. ► They are the first two examples of the solid materials containing {Mo5O16} chains.
Co-reporter:E. Yang, Zi-Sheng Liu, Shen Lin, Shun-Yu Chen
Inorganic Chemistry Communications 2011 Volume 14(Issue 10) pp:1588-1590
Publication Date(Web):October 2011
DOI:10.1016/j.inoche.2011.06.009
A porous metal organic framework [NiIIINiII2(μ3-OH)(bdc)1.5(int)3]n x(solvents) (1: bdc = 1,4-benzenedicarboxylate; int = isonicotinate) based on the trinuclear Ni3(μ3-OH) units was solvothermally synthesized and structurally characterized. It features a three-dimensional 9-connected ncb-type framework with two kinds of cage substructures and large one-dimensional channels. Both N2 and CO2 gas sorption studies of 1 were investigated to demonstrate the permanent porosity in 1.A microporous metal organic framework with 9-connected ncb topology is constructed from the trinuclear Ni3(μ3-OH) units and shows gas sorption properties.Research Highlights► Synthesis and structure of a microporous [Ni3(μ3-OH)] cluster-based framework ► Nine-connected ncb topology in metal organic framework ► A microporous metal organic framework with N2 and CO2 gas sorption properties
Co-reporter:Ming-Xing Yang,, Shen Lin, Si-Ning Zheng, Xiao-Hua Chen, Li-Juan Chen
Inorganic Chemistry Communications 2010 Volume 13(Issue 9) pp:1043-1046
Publication Date(Web):September 2010
DOI:10.1016/j.inoche.2010.06.006
Co-reporter:Shen Lin, Li-Juan Chen, Hui-Hong Xu, Jiang-Bo Su, Hua Huang
Inorganic Chemistry Communications 2010 Volume 13(Issue 11) pp:1347-1349
Publication Date(Web):November 2010
DOI:10.1016/j.inoche.2010.07.033
Two 2D metal–organic frameworks (MOFs), {[Zn4(Hbbim)4(bbim)2] 2H2O}n (1) and [Cd2(Hbbim)2(bbim)]n (2) (H2bbim = 2,2′-bibenzimidazole) were obtained by solvothermal reaction and characterized by single crystal X-ray diffraction analysis. Different metal ions, Cd(II)/Zn(II), adopt very different coordination geometries though two title compounds both have a 2D honeycomb network with (6,3) topology. The frameworks of compounds 1 and 2 are stable below 360 °C and 475 °C, respectively. Solid-state luminescent spectroscopy of compound 2 exhibits an emission peak at 407 nm.Two 2D honeycomb network structure based on the connectivity of 2,2′-bibenzimidazole and corresponding d10 metal ions(Zn2+, Cd2+) with the same (6,3) topology but different coordination geometries.
Co-reporter:Yuexu Lin, Shen Lin, Minghong Luo, Jiaohua Liu
Materials Letters 2009 Volume 63(13–14) pp:1169-1171
Publication Date(Web):31 May 2009
DOI:10.1016/j.matlet.2009.02.020
Sulfur anion doped Zn2SnO4 was prepared by calcining the mixture of thiourea and spinel Zn2SnO4 at 300 °C under argon atmosphere and characterized by XRD, XPS and DRS. It was found that S2− was incorporated interstitially into the bulk phase of Zn2SnO4. After the doping of S2−, the band gap of Zn2SnO4 was sharply decreased to 2.7 eV compared with that of undoped Zn2SnO4 (~ 3.6 eV). The photocatalytic activity of S-doped Zn2SnO4 was enhanced for photodegradation of Rhodamine B (RhB) in aqueous solution under visible light irradiation.
Co-reporter:Ming-xing Yang, Shen Lin, Li-juan Chen, Xiao-feng Zhang, Hui-hong Xu
Inorganic Chemistry Communications 2009 Volume 12(Issue 6) pp:566-568
Publication Date(Web):June 2009
DOI:10.1016/j.inoche.2009.04.022
Co-reporter:Shen Lin, Jiebo Chen, Xiulan Weng, Liuyi Yang, Xinqin Chen
Materials Research Bulletin 2009 44(5) pp: 1102-1105
Publication Date(Web):
DOI:10.1016/j.materresbull.2008.10.011
Co-reporter:Shen Lin;Xiaofeng Zhang;Minghong Luo
Journal of Solid State Electrochemistry 2009 Volume 13( Issue 10) pp:1585-1589
Publication Date(Web):2009 October
DOI:10.1007/s10008-008-0735-8
A novel inorganic–organic hybrid compound constructed from copper(II)-monosubstituted polyoxometalate Na5PW11Cu(H2O)O39 (PW11Cu) and poly(amidoamine) (PAMAM) dendrimer was prepared at room temperature in an aqueous solution. The title compound PW11Cu/PAMAM was characterized by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and X-ray diffraction, indicating that the PW11Cu was chemically anchored to PAMAM. The compound was first used as a bulk-modifier to fabricate a chemically modified carbon paste electrode (CPE) by direct mixing. The PW11Cu/PAMAM bulk-modified CPE showed well-defined cyclic voltammograms with four redox couples in 0.2 M NaAc buffer solution and high electrocatalytic activity for the reduction of hydrogen peroxide and nitrite. Furthermore, the CPE revealed good stability due to the insolubility of the title compound and the interaction between PW11Cu and PAMAM.
Co-reporter:Xiao-Feng Zhang;Geng-Geng Luo;Chun-Lian Liu
Chinese Journal of Chemistry 2007 Volume 25(Issue 3) pp:
Publication Date(Web):5 MAR 2007
DOI:10.1002/cjoc.200790063
An inorganic-organic composite was prepared by poly(amidoamine) (PAMAM) dendrimer reacting with cobalt(II)-monosubstituted polyoxometalates Na5CoII(H2O)PW11O39 (PW11Co) in an aqueous solution. The hybrid composite PW11Co/PAMAM was characterized by FT-IR, UV-Vis diffuse reflectance spectra (DR-UV-Vis), XPS, XRD and TG/DTA, indicating that the PW11Co was chemically anchored to PAMAM. The morphologies of the title composite were characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The catalytic activity was evaluated by oxidation of isobutyraldehyde (IBA) to isobutyric acid (IBAc) in MeCN under mild conditions (20 °C, ambient pressure), showing that the title compound is a more effective and recoverable catalyst than corresponding PW11Co.
Co-reporter:Xiaofeng Zhang;Xinqing Chen;Jiebo Chen
Frontiers of Chemistry in China 2007 Volume 2( Issue 4) pp:419-421
Publication Date(Web):2007 October
DOI:10.1007/s11458-007-0079-4
Mesoporous aluminophosphate was prepared by using G4.0 poly(amido amine)dendrimer as a template and characterized by Fourier transform infrared spectrometer (FTIR), X-ray diffraction (XRD), transmission electron microscopy (TEM) and N2 adsorption/desorption methods. Results show that the title compound exhibits a typical mesoporous structure with the average pore size from 5 to 8 nm. The formation mechanism of the nanoporous structure using dendrimer as a template was also discussed.
Co-reporter:Ming-Xing Yang, Li-Juan Chen, Shen Lin, Xiao-Hua Chen and Hua Huang
Dalton Transactions 2011 - vol. 40(Issue 9) pp:NaN1872-1872
Publication Date(Web):2010/11/30
DOI:10.1039/C0DT00781A
Three inorganic–organic compounds based on [MoxOy]n− chains, [Ag4(3-pttz)2Mo3O10] (1) (3-pttz = 5-(3-pyridyl) tetrazolate), [Ag4(2-pttz)2Mo4O13] (2) (2-pttz = 5-(2-pyridyl) tetrazolate), and [Ag4(pzttz)2Mo4O13] (3) (pzttz = 5-(pyrazinyl) tetrazolate), have been self-assembled, accompanied by in situ formation processes of the 5-substituted tetrazolate ligands under hydrothermal condition. Compound 1 features a 3D framework composed of [Mo3O10]2− chains cross-linked by [Ag4(3-pttz)2]2+ belts. Compounds 2 and 3 reveal the 3D structures based on [Mo4O13]2− chains pillared by silver tetrazolate polymeric chains. The three title compounds represent the first three examples that the tetrazolate ligands are introduced into the backbones of the [MoxOy]n− anion chains.
Co-reporter:Xiaofeng Zhang, Xiaoying Wang, Lijuan Le, Ai Ma and Shen Lin
Journal of Materials Chemistry A 2015 - vol. 3(Issue 38) pp:NaN19276-19276
Publication Date(Web):2015/08/20
DOI:10.1039/C5TA04450B
Octahedral Fe3O4 crystals were prepared by a facile potentiostatic deposition approach. The as-prepared Fe3O4 exhibits high electrocatalytic activity toward the oxygen reduction reaction (ORR) and excellent stability. The unique octahedral structure provides a high density of active sites and facilitates the ORR via a dominant pathway of oxygen reduction to hydroxide.
Co-reporter:Zhongshui Li, Xiaomei Huang, Xiaofeng Zhang, Lian Zhang and Shen Lin
Journal of Materials Chemistry A 2012 - vol. 22(Issue 44) pp:NaN23607-23607
Publication Date(Web):2012/09/24
DOI:10.1039/C2JM35239G
The {PEI-GNs/PMo12}n composite films are prepared by an LBL electrostatic assembly technique, and their uniform and homogeneous traits have been verified by UV-vis and cyclic voltammetry. The {PEI-GNs/PMo12}n composite films are used as a novel catalyst support for electro-deposition of Pt particles in situ. Pt particles immobilizing on the surface of {PEI-GNs/PMo12}n composite films were confirmed by XPS, EDX, XRD and FE-SEM. The interesting seashell-like Pt micro–nano-clusters can be obtained when {2PEI-GNs/PMo12} composite films are used as catalyst supports. Pt-{PEI-GNs/PMo12}n composite films present good electrocatalytic activity regarding methanol oxidation and improved tolerance of CO. These results indicate that poly(ethyleneimine) functionalized graphene (PEI-GNs) preserves the superior electric conductivities of graphene sheets in the composite films, and the introduction of electroactive [PMo12O40]3− (PMo12) into the composite films helps to convert intermediate species CO into CO2 from the Pt nanoparticles. The synergistic effect of PEI-GNs and PMo12 remarkably enhanced the electrocatalytic activity and stability regarding methanol oxidation.
Co-reporter:Lingting Ye, Zhongshui Li, Xiaofeng Zhang, Fengling Lei and Shen Lin
Journal of Materials Chemistry A 2014 - vol. 2(Issue 48) pp:NaN21019-21019
Publication Date(Web):2014/10/13
DOI:10.1039/C4TA05094K
A facile one-pot method was used to synthesize Pt/Cu2O/GNs and Pd/Cu2O/GNs composites. Pt or Pd nanoparticles are deposited onto graphene sheets (GNs) and Cu2O via synchronous reduction of K2PtCl4 (K2PdCl4), Cu(OH)2 and graphene oxide (GO) with glucose as a reducing agent under microwave irradiation. The formation of Cu2O promotes the nucleation of Pt(0) or Pd(0) particles and favors more complete reduction of PtCl42− or PdCl42−. Catalytic properties of as-prepared composites for methanol oxidation reaction (MOR) were evaluated by cyclic voltammetry (CV), chronoamperometry, COads stripping voltammetry and electrochemical impedance spectrum (EIS). Electrochemical experiments showed that Pt/Cu2O/GNs and Pd/Cu2O/GNs had much higher catalytic activity and stability for MOR and better resistance to CO poisoning compared with the commercially available Johnson Matthey 20% Pt/C catalyst (Pt/C-JM) and Sigma-Aldrich 20% Pd/C catalyst (Pd/C-SA). Especially under the UV irradiation, the total peak current density and catalytic stability of Pt/Cu2O/GNs and Pd/Cu2O/GNs drastically increase, which may result from the synergistic effect between the electro-catalytic and photo-catalytic properties. In brief, the cooperation among Pt (Pd), Cu2O and GNs promotes remarkably the catalytic performance for MOR on Pt/Cu2O/GNs and Pd/Cu2O/GNs either without light or with UV irradiation.
Co-reporter:Li-Juan Chen, Jiang-Bo Su, Rong-Bin Huang, Shen Lin, Ming-Xing Yang and Hua Huang
Dalton Transactions 2011 - vol. 40(Issue 38) pp:NaN9736-9736
Publication Date(Web):2011/08/22
DOI:10.1039/C1DT10723B
A 2D tri-layer compound {[Co8(tbip)6(H2O)9(OH)4]·12(H2O)}n (1) (H2tbip = 5-tert-butyl isophthalic acid) consisting of novel heptacobaltate clusters and single cobalt centers bridged by tbip2− ligands has been hydrothermally synthesized. The complex represents a rare example of a homometallic coordination polymer built up from both heptanuclear metal clusters and single metal centers simultaneously. The magnetic investigation reveals that the complex exhibits the overall predominance of antiferromagnetic coupling between magnetic centers.