Controllable photooxidation of 1-phenylethanol integrated with hydrogen evolution by a polyoxometalate/ZnIn_(2)S_(4)/WO_(3)catalytic system  

作　　者：Jiaxin Yang Yongkang Liu Yun Qin Zhenheng Diao Yuanyuan Dong Hongjin Lv 

机构地区：[1]School of Chemical Engineering,Advanced Institute of Materials Science,Changchun University of Technology,Changchun 130012,China [2]MOE Key Laboratory of Cluster Science,Beijing Key Laboratory of Photoelectric/Electrophotonic Conversion Materials,School of Chemistry and Chemical Engineering,Beijing Institute of Technology,Beijing 102488,China

出　　处：《Nano Research》2025年第4期116-124,共9页纳米研究(英文版)

基　　金：the financial support from the National Natural Science Foundation of China(Nos.22008012 and 22471019);the Hebei Natural Science Foundation(No.B2024105003);Development and Reform Commission Project of Jilin Province(No.2024C020-2);the Recruitment Program of Global Experts(Young Talents);BIT Excellent Young Scholars Research Fund.

摘　　要：The photocatalytic oxidation of 1-phenylethanol coupling with hydrogen evolution represents a promising strategy for the full utilization of the photogenerated electrons and holes to accomplish the maximum conversion of solar energy into chemical energy.To date,however,the controllable of reaction path and product distribution has yet not to be unrevealed.Herein,we report an efficient coupled catalytic system composed of ZnIn_(2)S_(4)/WO_(3)S-scheme heterojunction and Ni-containing polyoxometalate([Ni_(4)(H_(2)O)_(2)(PW_(9)O_(34))_(2)]^(10-)(Ni_(4)P_(2))),which exhibited excellent photocatalytic activities towards the oxidation valorization of 1-phenylethanol coupling with hydrogen evolution.The addition of Ni_(4)P_(2)can efficiently control the product distribution.Specifically,1-phenylethanol was preferentially converted to pinacol(86.0% selectivity)via C-C coupling over ZnIn_(2)S_(4)/WO_(3)S-scheme heterojunction accompanied by hydrogen production(202.4μmol),whereas it would be converted to acetophenone(93.8% selectivity)by photogenerated holes with concomitant hydrogen formation(183.1μmol)over the coupled Ni_(4)P_(2)/ZnIn_(2)S_(4)/WO_(3) catalytic system.Mechanism studies revealed that the hydrogen evolution cocatalyst Ni4P2,with its excellent electron storage capacity,can compete with the oxidation product acetophenone for electrons,and thus its addition can significantly inhibit the reduction of acetophenone,resulting in the inability to generate the coupling product pinacol.

关 键 词：S-scheme heterojunction ZnIn_(2)S_(4) POLYOXOMETALATES DEHYDROCOUPLING hydrogen evolution photocatalysis 

分 类 号：O643.36[理学—物理化学] O643.3[理学—化学]