Efficient Photocatalytic Hydrogen Evolution by Modulating Excitonic Effects in Ni-Intercalated Covalent Organic Frameworks

Rongchen Shen; Xiuzhi Li; Chaochao QinPeng ZhangXin Li

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Efficient Photocatalytic Hydrogen Evolution by Modulating Excitonic Effects in Ni-Intercalated Covalent Organic Frameworks

机译：Efficient Photocatalytic Hydrogen Evolution by Modulating Excitonic Effects in Ni-Intercalated Covalent Organic Frameworks

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Covalent organic frameworks (COFs) as appealing platforms have receivedtremendous interest in the field of photocatalytic H_2 evolution owing to theirwell-defined structures and tailor-made function. However, excitonic effectsresulting from Coulomb interactions between electron–hole pairs are key ratedeterminingprocesses in photocatalytic hydrogen evolution, which are usuallyignored. Thus, it is of profound significance and highly desired, but it isstill a challenge, to explore new routes to modulate excitonic dissociation inCOFs for boosting photocatalysis. To address this challenge, Ni-intercalatedfluorenone-based COFs (Ni-COF-SCAU-1) at the imine linkage, are proposedfor the first time, and demonstrated to exhibit the enhanced polarizationelectric field; thus, facilitating the Hall electron mobility and the dissociationof singlet excitons into free charge carriers under photoexcitation toparticipate in the surface hydrogen evolution reaction. Benefiting fromthese results, Ni-COF-SCAU-1 displays a hydrogen production rate of197.46 mmol·g~(?1) h~(?1) under visible light irradiation with an apparent quantumefficiency (AQE) up to 43.2% at 420 nm. This work offers an in-depth understandingof the crucial role of the interlayer atomic interface in improvingphotocatalytic hydrogen evolution and paves a new way for excitonic regulationin the COFs.

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来源
《Advanced energy materials》 |2023年第13期|2203695.1-2203695.11|共11页
作者
Rongchen Shen; Xiuzhi Li; Chaochao QinPeng ZhangXin Li;
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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;

Institute of Biomass EngineeringKey Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642, China,Henan Key Laboratory of Infrared Materials and SpectrumMeasures and;

Henan Key Laboratory of Infrared Materials and SpectrumMeasures and ApplicationsSchool of PhysicsHenan Normal UniversityXinxiang 453007, ChinaState Centre for International Cooperation on DesignerLow-Carbon & Environmental Materials (CDLCEM)School of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001, P. R. China;

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正文语种英语
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charge separation; exciton dissociation; Ni-intercalated COFs; photocatalytic hydrogen evolution; polarization electric field;

Efficient Photocatalytic Hydrogen Evolution by Modulating Excitonic Effects in Ni-Intercalated Covalent Organic Frameworks

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