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Accelerating solar driven CO_(2) reduction via sulfur-doping boosted water dissociation and proton transfer

查看全文 作　　者：Ke [1]Yan;Liang [2]Chen;Yangguang [3]Hu;Ting [1]Wang;Cong [1]Chen;Chao [3]Gao;Youju [2]Huang;Benxia [1]Li 高影响力作者 机构地区：[1]School of Chemistry and Chemical Engineering,Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang Province,Zhejiang Sci-Tech University,Hangzhou 310018,China;[2]College of Material,Chemistry and Chemical Engineering,Key Laboratory of Organosilicon Chemistry and Material Technology,Ministry of Education,Hangzhou Normal University,Hangzhou 311121,China;[3]School of Chemistry and Materials Science,University of Science and Technology of China,Hefei 230026,China高影响力机构 出　　处：《Nano Research》索引2024年第17卷第3期,共10页高影响力期刊 基　　金：supported by the Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(No.LZY23B030006);the Natural Science Foundation of Zhejiang Province of China(No.LY19B010005);the Fundamental Research Funds of Zhejiang Sci-Tech University(No.2020Y003). 摘　　要：Exploring efficient photocatalysts for solar driven CO_(2) reduction with water(H_(2)O)as a proton donor is highly imperative but remains a great challenge because the synchronous enhancement of CO_(2) activation,H_(2)O dissociation and proton transfer is hardly achieved on a photocatalyst.Particularly,the sluggish H_(2)O dissociation impedes the photocatalytic CO_(2) reduction reaction involving multiple proton–electron coupling transfer processes.Herein,a sulfur-doped BiOCl(S-BiOCl)photocatalyst with abundant oxygen vacancies(OV)is developed,which exhibits broadband-light harvesting across solar spectrum and distinct photothermal effect due to photochromism.For photocatalytic CO_(2) reduction with H_(2)O in a gas–solid system,the high CO yield of 49.76μmol·g_(cat)^(-1)·h^(-1) with 100%selectivity is achieved over the S-BiOCl catalyst under a simulated sunlight.The H_(2)O-assisted CO_(2) reduction reaction on S-BiOCl catalyst is triggered by photocatalysis and the photothermal heating further enhances the reaction rate.The kinetic isotope experiments indicate that the sluggish H_(2)O dissociation affects the whole photocatalytic CO_(2) reduction process.The presence of oxygen vacancies promotes the adsorption and activation of H_(2)O and CO_(2),and the doped S sites play a crucial role in boosting H_(2)O dissociation and accelerating the dynamic migration of hydrogen species.As a result,the ingenious integration of OV defects,S sites and photothermal effect in S-BiOCl catalyst conjointly contributes to the significant improvement in photocatalytic CO_(2) reduction performance. 关 键 词：BiOCl sulfur doping photocatalytic CO_(2)reduction H_(2)O activation proton feeding
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