Covalent Organic Framework (COF) derived Ni‐N‐C Catalysts for Electrochemical CO2 Reduction: Unraveling Fundamental Kinetic and Structural Parameters of the Active Sites

Changxia Li, Wen Ju*, Sudarshan Vijay, Janis Timoshenko, Kaiwen Mou, David A. Cullen, Jin Yang, Xingli Wang, Pradip Pachfule, Sven Brückner, Hyo Sang Jeon, Felix T. Haase, Sze-Chun Tsang, Clara Rettenmaier, Karen Chan, Beatriz Roldan Cuenya, Arne Thomas*, Peter Strasser*

*Corresponding author for this work

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Abstract

Electrochemical CO2 reduction is a potential approach to convert CO2 into valuable chemicals using electricity as feedstock. Abundant and affordable catalyst materials are needed to upscale this process in a sustainable manner. Nickel-nitrogen-doped carbon (Ni-N-C) is an efficient catalyst for CO2 reduction to CO, and the single-site Ni−Nx motif is believed to be the active site. However, critical metrics for its catalytic activity, such as active site density and intrinsic turnover frequency, so far lack systematic discussion. In this work, we prepared a set of covalent organic framework (COF)-derived Ni-N-C catalysts, for which the Ni−Nx content could be adjusted by the pyrolysis temperature. The combination of high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure evidenced the presence of Ni single-sites, and quantitative X-ray photoemission addressed the relation between active site density and turnover frequency.
Original languageEnglish
Article number e2021147
JournalAngewandte Chemie International Edition
Volume61
Number of pages9
ISSN1433-7851
DOIs
Publication statusPublished - 2022

Keywords

  • Active site density
  • CO2 reduction
  • Covalent organic framework
  • Single-site Ni-N-C
  • Turnover frequency

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