在水中生成H2的多功能光催化系统基于高效的DuBois型催化剂
Manuela A Gross1, Anna Reynal, James R Durrant
1Christian Doppler Laboratory for Sustainable SynGas Chemistry, Department of Chemistry, University of Cambridge , Lensfield Road, Cambridge CB2 1EW, U.K.
Journal of the American Chemical Society
|December 11, 2013
概括
一种新的- (NiP) 分子催化剂有效地利用光从水中产生 (H2). 这种催化剂在溶液和半导体表面都表现出高活性,为多功能可再生生产铺平了道路.
科学领域:
- 光催化作用的光催化
- 可再生能源可再生能源是可再生能源.
- 催化剂是一种催化剂.
- 绿色化学 绿色化学
背景情况:
- 有效的光化学 (H2) 生产需要有效的光诱导电子转移 (ET) 从光收割机到水中的电催化剂.
- 分子催化剂为优化催化过程提供可调节的特性.
研究的目的:
- 开发和描述一个具有增强水溶性和半导体固定能力的分子演化催化剂 (NiP).
- 在各种环境中研究光催化H2生成的光收割机 (RuP) 和NiP催化剂之间的电子转移的效率和机制.
主要方法:
- 电化学研究,以评估催化活性 (过电,法拉代收益率).
- 使用化Ru(II) tris(bipyridine) 染料 (RuP) 作为轻度收割机的光催化实验.
- 时间分辨率发光和短暂吸收光谱学研究电子转移动力学和通路.
主要成果:
- 尼催化剂在水溶液中表现出高的电催化活性 (200mV超电位,85%的法拉代产量).
- 从RuP到NiP的高效定向电子转移通过减少或氧化火观察到纳米到微秒的时间尺度.
- 高周转频率 (TOF) 为460±60h-1和周转数 (TON) 为723±171在均质的光催化H2生成中实现,光子对H2的量子收益率为~10%.
结论:
- P催化剂具有很高的多功能性,在纯水溶液中有效工作,并在半导体表面 (ZrO2,TiO2) 固定时有效工作.
- 该研究阐明了不同的电子转移路径,使高效的光催化H2生产成为可能.
- 这项工作为高效和多功能可再生产生提供了一个有希望的分子催化剂.
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