单核钌催化剂化学催化和光催化水氧化反应

doi:10.1016/S1872-2067(12)60600-7

催化学报 ›› 2013, Vol. 34 ›› Issue (8): 1489-1495.DOI: 10.1016/S1872-2067(12)60600-7

单核钌催化剂化学催化和光催化水氧化反应

姜毅^a, 李斐^a, 黄芳^a, 张彪彪^a, 孙立成^a,b

a 大连理工大学环境与生命科学学院, 精细化工国家重点实验室, 辽宁大连116024;
b 瑞典皇家工学院化学科学与工程学院化学系, 瑞典斯德哥尔摩10044

收稿日期:2013-03-22 修回日期:2013-04-10 出版日期:2013-08-16 发布日期:2013-07-30
通讯作者: 李斐,孙立成
基金资助:
国家自然科学基金(21106015,21120102036,20923006);国家重点基础研究发展计划(973计划, 2009CB220009);高等学校博士学科点专项科研基金(20110041120005);瑞典能源部K&A Wallenberg基金.

Chemical and photocatalytic water oxidation by mononuclear Ru catalysts

Yi Jiang^a, Fei Li^a, Fang Huang^a, Biaobiao Zhang^a, Licheng Sun^a,b

a State Key Laboratory of Fine Chemicals, Faculty of Chemical, Environmental and Biological Science and Technology, Dalian University of Technology, Dalian 116024, Liaoning, China;
b Department of Chemistry, School of Chemical Science and Engineering, KTH Royal Institute of Technology, Stockholm 10044, Sweden

Received:2013-03-22 Revised:2013-04-10 Online:2013-08-16 Published:2013-07-30
Supported by:
This work was supported by the National Basic Research Program of China (973 Program, 2009CB220009), the National Natural Science Foundation of China (21106015, 21120102036, and 20923006), the Research Fund for the Doctoral Program of Higher Education of China (20110041120005), and the Swedish Energy Agency and K&A Wallenberg Foundation.

摘要/Abstract

摘要： 合成了一系列含有不同对位取代基团的吡啶轴向配体的单核钌化合物Ru(bda)(pic)₂ (H₂bda=2,2'-联吡啶-6,6'-二羧酸; pic=对甲基吡啶),对化合物的结构进行了核磁、质谱和X射线单晶衍射表征,并在中性和酸性条件下研究了这些化合物的电化学性质.以硝酸铈铵为氧化剂,对催化剂的催化活性进行了测试,并以[Ru(bpy)₃]²⁺为光敏剂,S₂O₈^2-为电子牺牲剂,在三组分体系中考察了这些化合物的光催化活性.研究发现,在化学法水氧化反应中,化合物1由于其轴向配体4,4'-联吡啶在酸性条件下能够发生质子化,从而增强了吸电子效应,因此表现出最高的催化活性,催化循环数达到4000.在光催化水氧化反应中,化合物2因其轴向配体具有最强的吸电子能力而表现出最高的催化活性,反应2h的催化循环数达到270.结果表明,轴向配体的吸电子能力明显提高了这类Ru催化剂催化水氧化反应活性.

关键词: 分解水, 水氧化, 钌配合物, 吸电子效应, 光催化

Abstract: Four mononuclear Ru complexes with different substituents on the para position of the pyridine ligand of Ru(bda)(pic)₂ (H₂bda=2,2'-bipyridine-6,6'-dicarboxylic acid; pic=picoline) were synthesized and characterized by ¹H nuclear magnetic resonance or X-ray crystallography. The electrochemical properties of this series of compounds in acidic and neutral conditions were studied by cyclic voltammetry. Their catalytic activity towards water oxidation was investigated using a chemical oxidant ([Ce(NH₄)₂(NO₃)₆] (Ce^IV) in acidic solution, or driven by visible light in a three-component system containing a photosensitizer ([Ru(bpy)₃]²⁺) and an electron acceptor (S₂O₈^2-). For the chemical water oxidation, complex 1 was found to be the most effective, exhibiting a turnover number (TON) of up to 4000. The pyridine substituent at the 4-position in 1 may be protonated giving an intensive electron-withdrawing effect. Complex 2 bears the most electron-withdrawing trifluoromethyl group under neutral conditions and showed the highest photocatalytic activity with a TON of 270 over 2 h. It was concluded that the more electron-withdrawing substituents led to higher activity towards oxygen evolution for this type of Ru catalysts in the oxidation of water.

Key words: Water splitting, Water oxidation, Ruthenium complex, Electron-withdrawing effect, Photocatalysis

姜毅, 李斐, 黄芳, 张彪彪, 孙立成. 单核钌催化剂化学催化和光催化水氧化反应[J]. 催化学报, 2013, 34(8): 1489-1495.

Yi Jiang, Fei Li, Fang Huang, Biaobiao Zhang, Licheng Sun. Chemical and photocatalytic water oxidation by mononuclear Ru catalysts[J]. Chinese Journal of Catalysis, 2013, 34(8): 1489-1495.

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单核钌催化剂化学催化和光催化水氧化反应

Chemical and photocatalytic water oxidation by mononuclear Ru catalysts

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