Engineering β-ketoamine covalent organic frameworks for photocatalytic overall water splitting

Yan Yang, Xiaoyu Chu, Hong-Yu Zhang, Rui Zhang, Yu-Han Liu, Feng-Ming Zhang (), Meng Lu, Zhao-Di Yang () and Ya-Qian Lan ()
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Yan Yang: Harbin University of Science and Technology
Xiaoyu Chu: Harbin University of Science and Technology
Hong-Yu Zhang: Harbin University of Science and Technology
Rui Zhang: Harbin University of Science and Technology
Yu-Han Liu: Harbin University of Science and Technology
Feng-Ming Zhang: Harbin University of Science and Technology
Meng Lu: South China Normal University
Zhao-Di Yang: Harbin University of Science and Technology
Ya-Qian Lan: South China Normal University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Covalent organic frameworks (COFs) are an emerging type of crystalline and porous photocatalysts for hydrogen evolution, however, the overall water splitting activity of COFs is rarely known. In this work, we firstly realized overall water splitting activity of β-ketoamine COFs by systematically engineering N-sites, architecture, and morphology. By in situ incorporating sub-nanometer platinum (Pt) nanoparticles co-catalyst into the pores of COFs nanosheets, both Pt@TpBpy-NS and Pt@TpBpy-2-NS show visible-light-driven overall water splitting activity, with the optimal H2 and O2 evolution activities of 9.9 and 4.8 μmol in 5 h for Pt@TpBpy-NS, respectively, and a maximum solar-to-hydrogen efficiency of 0.23%. The crucial factors affecting the activity including N-sites position, nano morphology, and co-catalyst distribution were systematically explored. Further mechanism investigation reveals the tiny diversity of N sites in COFs that induces great differences in electron transfer as well as reaction potential barriers.

Date: 2023
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DOI: 10.1038/s41467-023-36338-x

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