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Citation: WANG Mingyan, XU Xingyou, MA Weixing, CAO Zhiling, YANG Xujie. Synthesis,Crystal Structure and Electrocatalytic Properties of a Tetranuclear Copper Cluster Complex[Cu₄(Pyims)₄]·4H₂O·4CH₃OH[J]. Chinese Journal of Applied Chemistry, ;2011, 28(3): 290-296. doi: 10.3724/SP.J.1095.2011.00282 shu

Synthesis,Crystal Structure and Electrocatalytic Properties of a Tetranuclear Copper Cluster Complex[Cu₄(Pyims)₄]·4H₂O·4CH₃OH

WANG Mingyan ^a,b ,
XU Xingyou ^b,c,, ,
MA Weixing ^b ,
CAO Zhiling ^b ,
YANG Xujie ^a

1.
a School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing;
2.
b Department of Chemical Engineering, Huaihai Institute of Technology, Lianyungang 222005;
3.
c Huaiyin Insititute of Technology, Huaiyin 223003

Corresponding author: XU Xingyou,
Received Date: 13 May 2010
Available Online: 18 July 2010
Fund Project: 国家自然科学基金(50873042) (50873042)江苏省海洋资源开发研究院科技开放基金(JSIMR09B05) (JSIMR09B05)江苏省自然科学基金(BK2009651)资助项目 (BK2009651)

A tetranuclear cluster crystal[Cu₄ (Pyims) ₄] ·4H₂O·4CH₃OH was synthesized from the reaction between cupric perchlorate and 4-(3-pyridyl) -2-mercapto imidazole(PyimsH) in methanol medium at room temperature, and characterized by elemental analysis, IR and single-crystal X-ray diffraction. The results reveal that the compound belongs to tetragonal system with space group I4₁/a. The cell parameters are a=1.44432(12) nm, b=1.44432(12) nm, c=2.2119(3) nm, α=90°, β=90°, γ=90°, V=4.6142(8) nm³, Z=4, D_c=1.669 Mg/m³, M_r=1159.26, R₁=0.0761, wR₂=0.1839(I >2σ). In the cluster molecule, the Cu₄⁴⁺ core takes a distorted tetrahedron configuration. Four Pyims^- ligands coordinate with cuprous ions by N atom of imidazole and S atom of sulfhydryl, and two cuprous ions are linked by one S atom t. The cluster molecules are held together via the N(3)----H(7)——C(7) hydrogen-bondings, which result in a three-dimensional network geometry. The electrochemical behavior of the title cluster was studied by cyclic voltammetry. Through simple dropcoating method, the title cluster was used to modify the surface of glassy carbon electrode(GCE) to fabricate an amperometric sensor. It has been found that the peak potential of the oxygen reduction at the modified electrode is positively shifted from -0.55 V to -0.247 V in pH=5.9 phosphate buffer solution. The obvious decrease of the over potential indicates that the sensor has high electrocatalytic activity to oxygen reduction, which suggests that the title cluster complex can be used as the anode material for fuel cells.
- copper cluster,
- synthesis,
- crystal structure,
- electrocatalysis,
- oxygen
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Synthesis,Crystal Structure and Electrocatalytic Properties of a Tetranuclear Copper Cluster Complex[Cu4(Pyims)4]·4H2O·4CH3OH

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通讯作者: 陈斌, bchen63@163.com

Synthesis,Crystal Structure and Electrocatalytic Properties of a Tetranuclear Copper Cluster Complex[Cu₄(Pyims)₄]·4H₂O·4CH₃OH