Revealing the electron transfer mechanism of defective carbon nitride during photocatalytic H_(2)O_(2)productionOA
Photosynthesis is a promising method for H_(2)O_(2)production,but its application in pure water is limited by slow oxidation kinetics and rapid photocarrier recombination of photocatalysts.Herein,a novel defective carbon nitride photocatalyst(D-C3-xN4)containing the C vacancies and the frustrated Lewis pairs(B and N of cyano group)is designed for H_(2)O_(2)photosynthesis,and the role of C vacancies on the electron transfer mechanism during photocatalysis is systematically investigated.The D-C_(3-x)N_(4) exhibits a H_(2)O_(2)production rate of 140.1μmol·g^(-1)·h^(-1) in pure water,which is 87.6 times that of C_(3)N_(4).Such superior performance for H_(2)O_(2)photosynthesis is found to arise from the C vacancies and frustrated Lewis pairs(FLPs).The C vacancies have strong electron-trapping ability,which greatly enhances the separation of photocarriers.The C vacancies can also effectively reduce O_(2)to*OOH via a proton-coupled process,which significantly accelerates the O_(2)reduction kinetics.Meanwhile,the FLPs show an outstanding catalytic activity for H_(2)O oxidation.This study not only provides a new structure for highly active photocatalysts,but also deepens the understanding of the electron transfer mechanism of photocatalysts with trapped sites.
Lixia Ma;Lu Zhang;Xiaojie Zhou;Jie Yang;Deng Li;Xuqian Zhao;Yinuo Su;Yu Chen;Zong-Huai Liu;Ruibin Jiang
Key Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,ChinaKey Laboratory of Applied Surface and Colloid Chemistry(Ministry of Education),Shaanxi Key Laboratory for Advanced Energy Devices,Shaanxi Engineering Lab for Advanced Energy Technology,School of Materials Science and Engineering,Shaanxi Normal University,Xi’an 710119,China
化学化工
hydrogen peroxide photosynthesisfemtosecond transient absorption spectroscopy(fs-TAS)defective carbon nitridecarbon vacancyfrustrated Lewis pairs
《Nano Research》 2026 (1)
P.233-243,11
supported by the Shaanxi Sanqin Scholars Innovation Team,the Science and Technology Project of Yan’an City(No.2023-CYL-193)the Key Science Research Plan of Department of Education in Shaanxi Province(No.23JS070)the Science Research Training Project(No.CLXZ2207).
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