物理化学学报2025,Vol.41Issue(9):146-157,12.DOI:10.1016/j.actphy.2025.100107
增强g-C3N4@BN范德华异质结界面上的三重态电子转移增强光催化合成H2O2
Enhanced photocatalytic synthesis of H2O2 by triplet electron transfer at g-C3N4@BN van der Waals heterojunction interface
摘要
Abstract
The van der Waals heterojunctions demonstrate exceptional advantages due to their outstanding charge separation capabilities and remarkable flexibility in tuning electronic properties.This study explores the potential application of the 2D/2D g-C3N4@BN van der Waals heterojunction in the photocatalytic synthesis of hydrogen peroxide(H2O2).Based on this heterojunction,we investigated the energy transfer process between triplet excitons and singlet oxygen,emphasizing the importance of catalyst structure for charge separation and the stable generation of triplet electrons.By constructing a charge transfer pathway,the built-in electric field within the heterojunction effectively drives the directional migration of charge carriers,significantly extending their lifetime.We employed two modification strategies to regulate the excited state electronic properties of the catalyst,including adjusting the interlayer arrangement to enhance charge transport capability and halogen modification to improve the light responsiveness of materials.Experimental validation indicates that the representative chlorinated-CN@BN effectively suppresses exciton recombination compared to CN,extending the lifetime of excited-state carriers by 3.52 times.Furthermore,the photocatalytic yield of H2O2 is improved by 2.73 times.This study provides a theoretical basis for developing novel photocatalysts and inspires the design of catalysts for direct synthesis of H2O2 from oxygen.关键词
2D/2D异质结界面/光催化合成H2O2/三重态电子转移/能量转移Key words
2D/2D heterojunction interface/Photocatalytic synthesis of H2O2/Triplet electron transfer/Energy transfer分类
化学化工引用本文复制引用
吴琦,王长华,李莹莹,张昕彤..增强g-C3N4@BN范德华异质结界面上的三重态电子转移增强光催化合成H2O2[J].物理化学学报,2025,41(9):146-157,12.基金项目
This work was supported by the Jilin Province Science and Technology Development Project(20220201073GX),the Natural Science Foundation of China(52273236,U22A2078,91833303,51102001),the Fundamental Research Funds for the Central Universities(2412022QD035),and the Education Department of Jilin Province(JJKH20241426KJ). 吉林省科技发展计划项目(20220201073GX)和国家自然科学基金(52273236,U22A2078,91833303,51102001),中央高校基本科研业务费专项资金(2412022QD035)和吉林省教育厅(JJKH20241426KJ)资助 (20220201073GX)