物理化学学报2025，Vol.41Issue(6)：91-102,12.DOI:10.1016/j.actphy.2025.100064
S型ZnO/CdIn2S4光催化剂制备H2O2偶联苄胺氧化的超快电子转移飞秒吸收光谱研究
Femtosecond transient absorption spectroscopy investigation on ultrafast electron transfer in S-scheme ZnO/CdIn2S4 photocatalyst for H2O2 production and benzylamine oxidation
摘要
Abstract
Photocatalytic hydrogen peroxide(H2O2)production is a crucial process for clean energy conversion,involving the reduction of O2 through two electrons.However,this process is often hampered by the sluggish water oxidation involving the photogenerated holes.To address this challenge,we have constructed a dual-functional S-scheme ZnO/CdIn2S4 heterojunction systerm coupling the H2O2 generation with a value-added benzylamine(BA)oxidation reaction.In this dual-functional photocatalytic system,photogenerated electrons in CdIn2S4 efficiently reduce O2 to produce H2O2,while photogenerated holes in ZnO selectively oxidize BA to N-benzylidenebenzylamine.Leveraging the advantages of the S-scheme heterojunction,the optimized ZnO/CdIn2S4 photocatalyst displays an enhanced H2O2 production rate(386 μmol·L-1·h-1)and BA oxidation fraction(81%)than pure ZnO or CdIn2S4.Femtosecond transient absorption(fs-TA)spectroscopy confirm the ultrafast S-scheme electron transfer from the ZnO conduction band(CB)to the CdIn2S4 valence band(VB)upon photoexcitation of the ZnO/CdIn2S4 composite.Besides,timely depletion of VB holes in ZnO and CB electrons in CdIn2S4 can accelerate the interfacial electron transfer in the ZnO/CdIn2S4 S-scheme heterojunction.The innovative design of the ZnO/CdIn2S4 S-scheme photocatalyst provides new insights for developing efficient dual-functional heterojunction photocatalytic systems and introduces a novel method for studying S-scheme heterojunctions using fs-TA spectroscopy.关键词
光催化产H2O2/S型异质结/选择性苄胺氧化/fs-TA光谱/电子转移动力学Key words
Photocatalytic H2O2 production/S-scheme heterojunction/Selective benzylamine oxidation/fs-TA spectroscopy/Electron transfer dynamics分类
化学化工引用本文复制引用
杨祎,周欣,谷苗莉,程蓓,吴珍,张建军..S型ZnO/CdIn2S4光催化剂制备H2O2偶联苄胺氧化的超快电子转移飞秒吸收光谱研究[J].物理化学学报,2025,41(6):91-102,12.基金项目
The project was supported by National Natural Science Foundation of China(22278324,52202375,22469001)and the Science Foundation of Hubei Province of China(2022CFA001).国家自然科学基金(22278324,52202375,22469001),湖北省自然科学基金(2022CFA001)资助项目 （22278324,52202375,22469001）
