室温下以4-(3-吡啶基)-2-巯基咪唑(PyiresH)和Cu(ClO4)2·6H2O为原料,在甲醇介质中制备了四核铜簇合物单晶[Cu4(Pyires)4]·4H2O-4CH3OH.该簇合物属四方晶系,14./a空间群.4个亚铜中心离子构成1个变形四面体,4个Pyims-配体以咪唑环上的N原子和巯基上的s原子与亚铜离子配位,其中S原子以桥基形式同时与2个亚铜离子配位.相邻簇合物分子通过配体Pyims-吡啶环上N3及C7之间的氢键交互作用,构筑成三维网状结构.采用简单的滴涂法将该簇合物修饰于玻碳电极表面,簇合物对O:气还原有良好的电催化活性,具有作为燃料电池电极材料的潜质.
参考文献
| [1] | YANG Hui,HUANG Zhizhong,JIANG Huijun,et al.Electrocatalytie Reduction of O2 and H2O2 at the Glass Carbon Electrode Modified with Mieroperoxidase-11[J].Acta Phys-Chim Sin,2000,16(6):527-532(in Chinese).杨辉,黄志忠.姜慧君,等.微过氧化物酶-11修饰电极对O2和H2O2的电催化还原[J].物理化学学报,2000,16(6):527-532. |
| [2] | LIU Shuqing,XU Jiqing,SUN Haoran,et al.Spectra and Eleetrocatalytic Reduction of Dioxygen of Meso-tetrakis(4-N-benzylpyridyl)porphyrin-metal-oxo Cluster Supramoleeular Complex[J].Acta Phys-Chim Sin,2001,17(2):128-131(in Chinese).刘淑清,徐吉庆,孙浩然,等.卟啉-金属氧簇超分子化合物的光谱及电催化氧还原[J].物理化学学报,2001,17(2):128-131. |
| [3] | DONG Shaojun,CHE Guangli,XIE Yuanwu.Chemical Modified Electrode[M].Beijing:Science Press,1995:216-219(in Chinese).董绍俊,车广礼,谢远武.化学修饰电极[M].北京:科学出版社,1995:216-219. |
| [4] | Brown A P,Koval C,Auson F C.Illustrative Electrochemical Behavior of Reactants Irreversibly Adsorbed on Graphite Electrode Surfaces[J].J Electroanal Chem,1976,72(3):379-384. |
| [5] | SU Haiquan,WU Bingfang,WANG Dingze.Synthesis and Crystal Structure of Triuclear Ruthenium Carbonyl Cluster with P,C1 Bridging Ligand[J].Chinese J lnorg Chem,2005,21(11):1727-1729(in Chinese).苏海全,吴秉芳,王丁泽.具有磷/氯桥基的三核钉羰基簇合物的合成和晶体结构[J].无机化学学报,2005,21(11):1727-1729. |
| [6] | LANG Jianping,XU Qingfeng,Jl Shunjun.Progress in the Synthesis and Structure Chemistry of Mo(W)/Cu(Ag)/S Clusters Derived with[Cp*MS3 J-[J].Chinese J Inorg Chem,2001,17(5):609-618(in Chinese).郎建平,徐庆锋,纪顺俊.含[Cp*MS,I-的钼(钨)/铜(银)/硫簇合物合成及结构化学的新进展[J].无机化学学报,2001,17(5).,609-618. |
| [7] | Shi S,Ji W,Tang S H,et al.Synthesis and Optical Limiting Capability of Cubane-like Mixed Metal Clusters(n-Bu4N)3[MoAg3BrX3S4](X＝Cl and I)[J].J Am Chem Soc,1994,116(8):3615-3616. |
| [8] | George R C,Thomas H,Grace C L.The Synthesis of Phenyl and Phridyl-glyoxalines[J].J Chem Soc,1938.23:753-758. |
| [9] | YI Hong,WANG Ting,XU Xiandong.Synthesis of 4-[4-(Pyridin-3-yl)imidazol-l-yl]Butanamine[J].Chinese J Pharm,2004,35:69-71(in Chinese).易红,王婷,许先栋.4-[4-(吡啶-3-基)咪唑-l-基]丁胺的合成[M].中国医药工业杂志,2004,35:69-71. |
| [10] | HU Yonglin,TANG Kaluo,TANG Youqi.Synthesis and Crystal Structure of Tetranuclear Copper Cluster Complex Cu4(C-C6Hl1CSS)4[J].Chinese J lnorg Chem,1992,S(2):103-109(in Chinese).胡永林,汤卡罗,唐有祺.四核铜原子簇化合物Cu4(c-C6H11CSS2)4的合成和结构研究[J].无机化学学报,1992,8(2):103-109. |
| [11] | Camus A,Marsich N,Manotti A M,et al.Insertion Reaction of Carbon Disulfide into Copper-carbon Bonds of Aromatic Organecopper(Ⅰ)Compounds,in the Presence of 2,2'-Bipyridine and 1,10-Phenanthroline.X-ray Diffraction Structures of the[(CuS3C-o-tolyl)phen],[(CuS3C-o-tolyl)2phen]and[Cu2(S3C-o-tolyl)(S2C-o-tolyl)bipy] Complexes[J].1norg Chim Acta[J],1990,175(2):193-198. |
| [12] | Schuennan J A,Fronczek F R,Selbin J.Selbin Crystal and Molecular Structures of Tetranuclear Medal Clusters of Copper(Ⅰ)Trithioperoxybenzoates[J].Inorg Chim Acta,1988,148(2):177-182. |
| [13] | Cai C X,Xue K H,Xu X Y,et al.Electrocatalysis for the Reduction of O2 and H2O2 Based on Complex of Copper(Ⅱ) with the Tris(3-aminopropyl)amine and Imidazole Ligands[J].J Appl Electrochem,1997,27:793-798. |
| [14] | Zhang Z Z,Auson F C.Electrocatalysts for the Reduction of O2 and H2O2 Based on Complexes of Cu(Ⅰ)with the Strongly Adsorbing 2,9-Dimethyl-1,10-phenanthroline Ligand[J].Electrochim Acta,1993,38:2423-2425. |
| [15] | XU Jingiuan,FANF Huiqun,CHEN Hongynan.The Electrochemical Characteristics of Gold Electrode Modified by Thionine Covalently Bound to Self-assembled Cysteamine Monolayer and Its Electrocatalytic Oxidation for Ascorbie Acid[J].Chem J Chinese Unw,1997,18:706-710(in Chinese).徐静娟,方惠群,陈洪渊.硫堇衍生化自组装膜修饰金电极的电化学性质厦其抗坏血酸的电催化氧化[J].高等学校化学学报,1997,18:706-710. |
| [16] | CHEN Zhen,YAO Jiannian.The Electrochemical Determination Method[M].Beijing:Peking University Press,1995:431-441(in Chinese).陈震,姚建年.电化学测定方法[M].北京:北京大学出版社,1995:431-441. |
| [17] | ZHA Quanxing.An Introduction to Electrode Kinetics[M].Beijing:Science Press,2002:271-275(in Chinese).查全性.电极过程动力学导论[M].北京:科学出版社,2002:271-275. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%