The Linkage‐Moderated Covalent Organic Frameworks with C=N and NN on Charge Transfer Kinetics Towards the Robust Photocatalytic Hydrogen Activity

Author:

Wu Haiyang1,He Xuan1ORCID,Du Xing1,Wang Daheng1,Li Weixin1ORCID,Chen Hui1,Fang Wei1,Zhao Lei1

Affiliation:

1. The State Key Laboratory of Refractories and Metallurgy Wuhan University of Science & Technology Wuhan 430081 P. R. China

Abstract

AbstractSince the linkages structured in covalent organic frameworks (COFs) usually impact the charge transfer behavior during photocatalytic hydrogen evolution reaction (pc‐HER), linkage dependence on charge transfer kinetics should be further claimed. Herein, COFs with N‐based linkages and pyrene‐based building nodes are constructed to enable us to obtain new clues about the charge transfer behavior and evolution tendency relevant to linkages at a molecular level for pc‐HER. It is demonstrated that photo‐excited electrons preferably move to the N sites in C=N linkage for pc‐HER and are trapped around NN linkage as well. A high electron transfer rate does not point to high photocatalytic activity directly, while a small difference between the electron transfer rate and electron recombination rate ΔkCTCR predicts the inefficiency of charge transfer in Azod‐COFs. Contrarily, large value of ΔkCTCR in the case of Benzd‐COFs, demonstrats an unimpeded charge transfer process to result in boosted pc‐HER rate (2027.3 µmol h−1 g−1). This work offers a prominent strategy for the reasonable design of efficient photocatalysts at the molecular level for structural regulation and achieves an efficient charge transfer process for the pc‐HER process.

Funder

National Natural Science Foundation of China

Natural Science Foundation of Hubei Province

Wuhan University of Science and Technology

Publisher

Wiley

Subject

Biomaterials,Biotechnology,General Materials Science,General Chemistry

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