Photocatalytic hydrogen evolution by two comparable [FeFe]‐hydrogenase mimics assembled to the surface of ZnS
Photocatalytic hydrogen evolution by two comparable [FeFe]‐hydrogenase mimics assembled to the surface of ZnS
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DOI：
10.1002/aoc.3119
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发表时间：
2014-04
影响因子：
3.9
通讯作者：
Xiaowei Song;H. Wen;Cheng-Bing Ma;M. Hu;Hui Chen;Hong-hua Cui;Changneng Chen
中科院分区：
文献类型：
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作者：
Xiaowei Song;H. Wen;Cheng-Bing Ma;M. Hu;Hui Chen;Hong-hua Cui;Changneng Chen
在DMF-H_2 O（9/1，v/v）溶液中，以三乙醇胺为电子给体，将含羧基和不含羧基的[FeFe]-氢化酶模拟物（C1）组装到ZnS表面，构建了两种光催化析氢体系。辐照30 h后，C1/ZnS和C2/ZnS的析氢周转数分别为3400和4950。C2/ZnS体系的光催化活性比原始ZnS的活性高5倍，表明[FeFe]-氢化酶模拟物对提高ZnS的活性至关重要。根据光谱研究和分析，ZnS的光生电子转移到模拟物可能是负责的活性增强。产氢的时间依赖性表明，模拟C2比C1更活跃。不同的析氢活性可以归因于两种[FeFe]-氢化酶模拟物在ZnS表面的不同吸附模式。版权所有© 2014约翰威利父子有限公司.
Two photocatalytic hydrogen evolution systems were constructed by assembling [FeFe]-hydrogenase mimics, either carboxyl group-containing (C1) or not (C2), on to the surface of ZnS using triethanolamine as electron donor in DMF-H2O (9/1, v/v) solution. Upon irradiation for 30 h, the turnover numbers of hydrogen evolution were 3400 and 4950 for the hybrid system C1/ZnS and C2/ZnS, respectively. The photocatalytic activity of the C2/ZnS system was five times higher than the activity of the pristine ZnS, suggesting that the [FeFe]-hydrogenase mimics are crucial toward improving the activity of ZnS. On the basis of the spectroscopic studies and analyses, the photogenerated electron transfer from ZnS to the mimics is probably responsible for the activity enhancement of ZnS. The time dependence of hydrogen generation shows that the mimic C2 is more active than C1. The different hydrogen evolution activity can be attributed to the different adsorption modes of the two [FeFe]-hydrogenase mimics on the surface of ZnS. Copyright © 2014 John Wiley & Sons, Ltd.