Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis

Ziqi Zhang, Zhe Zhang, Cailing Chen, Rui Wang, Minggang Xie, Sheng Wan, Ruige Zhang, Linchuan Cong, Haiyan Lu (), Yu Han, Wei Xing (), Zhan Shi () and Shouhua Feng
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Ziqi Zhang: College of Chemistry, Jilin University
Zhe Zhang: College of Chemistry, Jilin University
Cailing Chen: Physical Sciences and Engineering Division, King Abdullah University of Science and Technology (KAUST)
Rui Wang: College of Chemistry, Jilin University
Minggang Xie: College of Chemistry, Jilin University
Sheng Wan: College of Chemistry, Jilin University
Ruige Zhang: College of Chemistry, Jilin University
Linchuan Cong: College of Chemistry, Jilin University
Haiyan Lu: College of Chemistry, Jilin University
Yu Han: South China University of Technology
Wei Xing: Changchun Institute of Applied Chemistry, Chinese Academy of Sciences
Zhan Shi: College of Chemistry, Jilin University
Shouhua Feng: College of Chemistry, Jilin University

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Two-dimensional (2D) covalent organic frameworks (COFs) and their derivatives have been widely applied as electrocatalysts owing to their unique nanoscale pore configurations, stable periodic structures, abundant coordination sites and high surface area. This work aims to construct a non-thermodynamically stable Pt-N2 coordination active site by electrochemically modifying platinum (Pt) single atoms into a fully conjugated 2D COF as conductive agent-free and pyrolysis-free electrocatalyst for the hydrogen evolution reaction (HER). In addition to maximizing atomic utilization, single-atom catalysts with definite structures can be used to investigate catalytic mechanisms and structure-activity relationships. In this work, in-situ characterizations and theoretical calculations reveal that a nitrogen-rich graphene analogue COF not only exhibits a favorable metal-support effect for Pt, adjusting the binding energy between Pt sites to H* intermediates by forming unique Pt-N2 instead of the typical Pt-N4 coordination environment, but also enhances electron transport ability and structural stability, showing both conductivity and stability in acidic environments.

Date: 2024
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DOI: 10.1038/s41467-024-46872-x

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