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Enhancing Photocatalytic Hydrogen Evolution through Electronic Structure and Wettability Adjustment of ZnIn_(2)S_(4)/Bi_(2)O_(3) S-Scheme Heterojunction

调控ZnIn_(2)S_(4)/Bi_(2)O_(3)S型异质结的电子结构和润湿性增强光催化析氢
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摘要 The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability. 通过光催化水裂解制氢来生产可再生燃料具有巨大的潜力。然而,缓慢的析氢动力学和较差的水吸附对光催化剂构成了重大挑战。在这项研究中,我们开发了一种简单的水热法,用于从金属有机框架(MOF)中合成Bi_(2)O_(3)(BO),并将其负载到花状ZnIn_(2)S_(4)(ZIS)上。该方法显著增强了水吸附和表面催化反应,从而显著提高了光催化活性。以三乙醇胺(TEOA)作为牺牲剂,在BO上负载15%(质量分数)ZIS时,析氢速率达到了1610μmol∙h^(−1)∙g^(−1),是纯BO的6.34倍。此外,利用密度泛函理论(DFT)和从头算分子动力学(AIMD)计算,我们确定了ZIS/BO S型异质结界面上的反应,包括水吸附和催化反应的活性位点。这项工作将为开发具有特定电子性能和润湿性的高性能复合光催化材料提供有价值的见解。
作者 Linfeng Xiao Wanlu Ren Shishi Shen Mengshan Chen Runhua Liao Yingtang Zhou Xibao Li 肖林锋;任婉璐;沈诗诗;陈梦姗;廖润华;周英棠;李喜宝(景德镇陶瓷大学材料科学与工程学院,江西景德镇333403;浙江海洋大学海洋科学与技术学院,浙江省石油化工环境污染控制重点实验室,国家海洋设施养殖工程技术研究中心,浙江舟山316022;南昌航空大学材料科学与工程学院,南昌330063)
出处 《物理化学学报》 SCIE CAS CSCD 北大核心 2024年第8期50-63,共14页 Acta Physico-Chimica Sinica
基金 浙江省重点研发项目(2023 C01191) 国家自然科学基金项目(22262024,51962023,51468024) 江西省重点学科学术技术带头人项目(20232BCJ22008) 江西自然科学基金(20232ACB204007,20202BABL203037) 景德镇市科技局项目(20192GYZD008-33)资助。
关键词 S-scheme Hydrogen evolution WETTABILITY PHOTOCATALYSIS Electronic structure S型 析氢 润湿性 光催化 电子结构
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