Journal Article PUBDB-2023-00412

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Covalent Organic Framework (COF) Derived Ni‐N‐C Catalysts for Electrochemical CO$_2$ Reduction: Unraveling Fundamental Kinetic and Structural Parameters of the Active Sites

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2022
Wiley-VCH Weinheim

Angewandte Chemie / International edition 61(15), e202114707 () [10.1002/anie.202114707]
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Abstract: Electrochemical CO$_2$ reduction is a potential approach to convert CO$_2$ 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 CO$_2$ 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.

Classification:

Contributing Institute(s):
  1. DOOR-User (DOOR ; HAS-User)
Research Program(s):
  1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
  2. DFG project 390540038 - EXC 2008: Unifying Systems in Catalysis "UniSysCat" (390540038) (390540038)
Experiment(s):
  1. PETRA Beamline P64 (PETRA III)

Appears in the scientific report 2022
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Medline ; Creative Commons Attribution CC BY 4.0 ; OpenAccess ; Chemical Reactions ; Clarivate Analytics Master Journal List ; Current Contents - Life Sciences ; Current Contents - Physical, Chemical and Earth Sciences ; DEAL Wiley ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 15 ; Index Chemicus ; JCR ; NationallizenzNationallizenz ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection
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 Record created 2023-01-20, last modified 2025-07-24


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