journal article·2022-06-14

Constructing Synergistic Triazine and Acetylene Cores in Fully Conjugated Covalent Organic Frameworks for Cascade Photocatalytic H2O2 Production

Lipeng Zhai, Zhipeng Xie, Cheng-Xing Cui, Xiubei Yang, Qing Xu, Xiating Ke, Minghao Liu, Ling-Bo Qu, Xiong Chen, Liwei Mi

Chemistry of Materials· Volume 34· Issue 11
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Abstract

Covalent organic frameworks (COFs) are an ideal template for photocatalytic H2O2 synthesis because of the tunable chemical structures and semiconductor properties. However, the photoactivity for COFs is still under-improved due to the inefficient intrinsic charge generation, fast recombination of photogenerated charges, and limited electron transport along the frameworks. Herein, spatially separated and synergistic triazine and acetylene units are first integrated into COFs (EBA-COF and BTEA-COF) for photocatalytic H2O2 production. The spatial separation of triazine and acetylene cores leads to efficient charge separation and suppressed charge recombination, and C═C linkage facilitates electrons transport over the skeletons. Both experimental and computational results suggested that triazine and acetylene units synergistically promote H2O2 synthesis in a two-electron pathway. The EBA-COF showed an attractive activity with a H2O2 production rate of 1830 μmol h–1 gcat–1, superior to that of most other COF-based catalysts. This study provides a method for designing photocatalysts with synergistic photocatalytic active sites based on vinylene-linked COFs.
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Research context

OpenAlex topics: Covalent Organic Framework Applications · Advanced Photocatalysis Techniques · Metal-Organic Frameworks: Synthesis and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Henan Key Laboratory of Functional Salt Materials, Center for Advanced Materials Research, Zhongyuan University of Technology, Zhengzhou 450007, P. R. China

State Key Laboratory of Photocatalysis on Energy and Environment, and Key Laboratory of Molecular Synthesis and Function Discovery, College of Chemistry, Fuzhou University, Fuzhou 350116, P. R. China

School of Chemistry and Chemical Engineering, Henan Institute of Science and Technology, Xinxiang 453003, P. R. China

CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute (SARI), Chinese Academy of Sciences (CAS), Shanghai 201210, P. R. China

College of Chemistry, and Institute of Green Catalysis, Zhengzhou University, Zhengzhou 450001, P. R. China

Funding

Natural Science Foundation of Shanghai · National Natural Science Foundation of China · Key Projects of Science and Technology of Henan Province · Program of Science and Technology Innovation Leading Talent of Zhongyuan

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