异腈氮杂配铜配合物的合成及光解水制氢性能
Aza-Isocyanide Heteroleptic Copper Complexes: Synthesis and Application in Photocatalytic Hydrogen Evolution From Water
作者单位E-mail
夏良敏 浙江工业大学绿色化学合成技术国家重点实验室培育基地, 杭州 310014  
陈浩 浙江工业大学绿色化学合成技术国家重点实验室培育基地, 杭州 310014  
吴庆安 浙江工业大学绿色化学合成技术国家重点实验室培育基地, 杭州 310014  
王肖璟 浙江工业大学义乌科学技术研究院, 义乌 322001  
娄文雅 浙江工业大学义乌科学技术研究院, 义乌 322001  
徐斌 浙江工业大学义乌科学技术研究院, 义乌 322001 xubin@zjut.edu.cn 
罗书平 浙江工业大学绿色化学合成技术国家重点实验室培育基地, 杭州 310014;浙江工业大学义乌科学技术研究院, 义乌 322001 Luoshuping@zjut.edu 
摘要: 设计、合成了供电子性能的异腈二齿配体,可与铜(Ⅰ)和1,10-菲咯啉衍生物发生反应,形成一类异腈氮杂配铜光敏剂4a~4h,并在光解水制氢体系研究了其光催化活性。实验结果表明,2,2'-二异腈基二苯硫醚与2,9位具有取代基的菲咯啉形成的杂配铜配合物具有一定的光敏活性,光解水制氢TON达168。结合这类配合物的光物理性能和光电性能研究,对这类配合物作为光敏剂的构效关系及其内在机理进行了初步地解释与探讨。
关键词: 异腈  杂配铜配合物  光敏剂  光解水  制氢
基金项目: 国家自然科学基金(No.21376222)资助项目。
Abstract: A electron-donating bidentate ligands of isocyano-compounds were designed and synthesized, which could formed a series of aza-isocyanide heteroleptic copper photosensitizers 4a~4h with 1, 10-phenanthroline derivatives as N ligands. The photosensitive activities of this copper complexes were studied in water reduction system, and the turnover number (TON) of hydrogen evolution was up to 168 with bis(2-isocyanophenyl)sulfane as isocyanide ligand and 1, 10-phenanthroline with 2, 9-disubstitutes as N ligand. After the photophysical and photoelectric properties of these copper complexes were studied, a preliminary explanation and discussion of the structure-activity relationship and the mechanism of photocatalytic hydrogen evolution from water were carried out.
Keywords: isocyanide  heteroleptic copper complexes  photosensitizer  water splitting  hydrogen evolution
投稿时间:2016-09-06 最后修改时间:2017-02-25
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夏良敏,陈浩,吴庆安,王肖璟,娄文雅,徐斌,罗书平.异腈氮杂配铜配合物的合成及光解水制氢性能[J].无机化学学报,2017,33(4):560-568.
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