title: Unraveling a Single-Step Simultaneous Two-Electron Transfer Process from Semiconductor to Molecular Catalyst in a CoPy/CdS Hybrid System for Photocatalytic H2 Evolution under Strong Alkaline Conditions.
abstract: 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.
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian National Laboratory for Clean Energy, Dalian 116023, China.|Graduate University of Chinese Academy of Sciences , Beijing 100049, China.|Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) , China.
authors.forename: Yuxing
authors.initials: Y
authors.lastname: Xu
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian National Laboratory for Clean Energy, Dalian 116023, China.|Graduate University of Chinese Academy of Sciences , Beijing 100049, China.|Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) , China.
authors.forename: Yun
authors.initials: Y
authors.lastname: Ye
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian National Laboratory for Clean Energy, Dalian 116023, China.|Graduate University of Chinese Academy of Sciences , Beijing 100049, China.|Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) , China.
authors.forename: Taifeng
authors.initials: T
authors.lastname: Liu
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian National Laboratory for Clean Energy, Dalian 116023, China.|Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) , China.
authors.forename: Xiuli
authors.initials: X
authors.lastname: Wang
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian National Laboratory for Clean Energy, Dalian 116023, China.
authors.forename: Bingqing
authors.initials: B
authors.lastname: Zhang
authors.affiliation: State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology , Dalian 116024, China.
authors.forename: Mei
authors.initials: M
authors.lastname: Wang
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian National Laboratory for Clean Energy, Dalian 116023, China.|Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) , China.
authors.forename: Hongxian
authors.initials: H
authors.lastname: Han
authors.affiliation: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian National Laboratory for Clean Energy, Dalian 116023, China.|Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) , China.
authors.forename: Can
authors.initials: C
authors.lastname: Li