Unraveling a Single-Step Simultaneous Two-Electron Transfer Process from Semiconductor to Molecular Catalyst in a CoPy/CdS Hybrid System for Photocatalytic H2Evolution under Strong Alkaline Conditions,Journal of the American Chemical Society

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Unraveling a Single-Step Simultaneous Two-Electron Transfer Process from Semiconductor to Molecular Catalyst in a CoPy/CdS Hybrid System for Photocatalytic H2Evolution under Strong Alkaline Conditions
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2016-08-18 , DOI: 10.1021/jacs.6b04080
Yuxing Xu _{1,

2,

3} , Yun Ye _{1,

2,

3} , Taifeng Liu _{1,

2,

3} , Xiuli Wang _{1,

3} , Bingqing Zhang ₁ , Mei Wang ₄ , Hongxian Han _{1,

3} , Can Li _{1,

3}

Affiliation

Electron transfer processes from semiconductor to molecular catalysts was studied in a model hybrid photocatalytic hydrogen evolution system composed of [Co((III))(dmgH)2PyCl] (CoPy) and CdS under different pH conditions. Thermodynamic and kinetic studies revealed that photocatalytic H2 evolution under high pH conditions (pH 13.5) can only account for the thermodynamically more favorable single-step simultaneous two-electron transfer from photoirradiated CdS to Co(III)Py to produce unavoidable intermediate Co(I)Py, rather than a two-step successive one-electron transfer process. This finding not only provides new insight into the charge transfer processes between semiconductors and molecular catalysts but also opens up a new avenue for the assembly and optimization of semiconductor-molecular catalyst hybrid systems processed through multielectron transfer processes.

中文翻译：

在强碱性条件下，在 CoPy/CdS 混合系统中解开从半导体到分子催化剂的单步同步双电子转移过程，用于光催化 H2 析出

在由 [Co((III))(dmgH)2PyCl] (CoPy) 和 CdS 组成的模型混合光催化析氢系统中，在不同 pH 条件下研究了从半导体到分子催化剂的电子转移过程。热力学和动力学研究表明，在高 pH 条件（pH 13.5）下光催化析氢只能解释热力学上更有利的单步同时双电子从光照射的 CdS 转移到 Co(III)Py 以产生不可避免的中间体 Co(I) Py，而不是两步连续的单电子转移过程。

更新日期：2016-08-18

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