文献类型：期刊文献

英文题名：Independent Optimization of the Redox Reaction Sites for Simultaneous Production of Value-Added Organic Compounds and Hydrogen with High Activity and Selectivity

作者：Liu, Weilong[1,2,3];Xu, Zehong[1,2,3];Liu, Cong[1,2];Li, Hao[1,2,3];Zhang, Mengjun[1,2,3];Wang, Lingzhi[1,2,3];Wu, Shiqun[1,2,3];Cao, Xiao-ming[1,2,3,4];Ye, Ziwei[1,2,3];Zhang, Jinlong[1,2,3]

机构：[1]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn,Key Lab Adv Mat, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Joint Int Res Lab Precis Chem & Mol Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalysi, Shanghai 200237, Peoples R China;[4]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China

年份：2026

卷号：16

期号：6

起止页码：5966

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20261220317849);WOS:【SCI-EXPANDED(收录号:WOS:001707629600001)】；

基金：This work was supported by the National Natural Science Foundation of China (22461142136, 22503031), the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Science and Technology Commission of Shanghai Municipality (20DZ2250400, 2018SHZDZX03), Shanghai Pujiang Program (No. 23PJ1401900), and Fundamental Research Funds for the Central Universities (222201717003).

语种：英文

外文关键词：photocatalytic organic synthesis; S-schemeheterojunction; localized surface plasmon resonance; photocatalytichydrogen evolution; directional charge transfer mechanism

摘要：Developing integrated photocatalytic systems for the simultaneous production of value-added organic compounds and hydrogen is a promising approach to efficient solar energy utilization. However, it also proves to be highly challenging, since it requires catalytic surface sites that are optimized for both photocatalytic oxidation and reduction reactions. Here, we addressed this challenge by constructing a hollow S-scheme heterojunction photocatalyst composed of hollow WO2.72 (WOHS) and CdS. The key benefit of this heterojunction is that it enabled directional charge transfer between WOHS and CdS, which allowed the reaction sites for oxidation and reduction reaction to be effectively separated from each other. Exploiting this advantage enabled further optimization of the oxidation and reduction reaction sites independently, which was achieved by depositing Ni and Co3O4 selectively on the CdS and WOHS surface. We demonstrated that this not only enhanced charge-separation efficiency but also significantly lowered the activity energy for proton reduction and center dot CH(OH)Ph radical dehydrogenation. The resulting heterojunction therefore exhibited high activity for hydrogen evolution and BA-to-BAD oxidation with selectivity that is unachievable with each of the component photocatalyst separately.