Heteroatom- and Bonded Z-Scheme Channels-Modulated Ultrafast Carrier Dynamics and Exciton Dissociation in Covalent Triazine Frameworks for Efficient Photocatalytic Hydrogen Evolution

Rongchen Shen; Neng Li; Chaochao QinXiuzhi LiPeng ZhangXin LiJunwang Tang

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Heteroatom- and Bonded Z-Scheme Channels-Modulated Ultrafast Carrier Dynamics and Exciton Dissociation in Covalent Triazine Frameworks for Efficient Photocatalytic Hydrogen Evolution

机译：Heteroatom- and Bonded Z-Scheme Channels-Modulated Ultrafast Carrier Dynamics and Exciton Dissociation in Covalent Triazine Frameworks for Efficient Photocatalytic Hydrogen Evolution

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Covalent triazine frameworks (CTF) offer a tunable platform for photocatalyticH_2 generation due to their diverse structures, low costs, and precisely tunableelectronic structures. However, high exciton binding energy and shortlifetimes of photogenerated carriers restrict their application in photocatalytichydrogen evolution. Herein, a novel phosphorus-incorporated CTF isintroduced to construct a chemically bonded PCTF/WO_3 (PCTFW)heterostructure with a precise interface electron transfer channel. Thephosphorus incorporation is found to dominantly reduce the exciton bindingenergy and promote the dissociation of singlet and triplet excitons into freecharge carriers due to the regulation of electronic structures. High-qualityinterfacial W–N bonds improve the interfacial transfer of photogeneratedelectrons, thus prolonging the lifetime of photogenerated electrons.Femtosecond transient absorption spectroscopy characterizations and DFTcalculations further confirm both phosphorus incorporation and Z-schemeheterojunctions can synergistically boost the in-built electric field andaccelerate the migration and separation of photogenerated electrons. Theoptimized photocatalytic H_2-evolution rate of resultant PCTFW is 134.84 μmolh~(?1) (67.42 mmol h~(?1)g~(?1)), with an apparent quantum efficiency of 37.63% at420 nm, surpassing many reported CTF-based photocatalysts so far. Thiswork highlights the significance of atom-level interfacial exciton dissociation,and charge transfer and separation in improving photocatalysis.

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《Advanced functional materials》 |2023年第34期|2301463.1-2301463.12|共12页
作者
Rongchen Shen; Neng Li; Chaochao QinXiuzhi LiPeng ZhangXin LiJunwang Tang;
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作者单位

Institute of Biomass EngineeringKey Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642, China;

State Key Laboratory of Silicate Materials for ArchitecturesWuhan University of TechnologyHubei 430070, China;

Henan Key Laboratory of Infrared Materials and Spectrum Measures andApplicationsSchool of PhysicsHenan Normal UniversityXinxiang, Henan 453007, ChinaState Centre for International Cooperation on Designer Low-Carbon &Environmental Materials (CDLCEM)School of Materials Science and EngineeringZhengzhou UniversityZhengzhou, Henan 450001, P. R. ChinaDepartment of Chemical EngineeringUniversity College LondonLondon WC1E 7JE, UK;

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正文语种英语
中图分类无线电电子学、电信技术;工程材料学;
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charge separation; exciton dissociation; phosphorus-incorporated covalent triazine frameworks; photocatalytic hydrogen evolution; Z-scheme heterojunctions;

Heteroatom- and Bonded Z-Scheme Channels-Modulated Ultrafast Carrier Dynamics and Exciton Dissociation in Covalent Triazine Frameworks for Efficient Photocatalytic Hydrogen Evolution

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