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

Li, C., Ju, W., Vijay, S., Timoshenko, J., Mou, K., Cullen, D. A., et al. (2022). Covalent Organic Framework (COF) derived Ni-N-C Catalysts for Electrochemical CO2 Reduction: Unraveling Fundamental Kinetic and Structural Parameters of the Active Sites. Angewandte Chemie International Edition, 61(15): e202114707. doi:10.1002/anie.202114707.

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Angew Chem Int Ed - 2022 - Li - Covalent Organic Framework COF Derived Ni%u2010N%u2010C Catalysts for Electrochemical CO2 Reduction.pdf (Publisher version), 2MB
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Angew Chem Int Ed - 2022 - Li - Covalent Organic Framework COF Derived Ni%u2010N%u2010C Catalysts for Electrochemical CO2 Reduction.pdf
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 Creators:
Li, Changxia1, Author
Ju, Wen2, Author
Vijay, Sudarshan3, Author
Timoshenko, Janis4, Author           
Mou, Kaiwen2, Author
Cullen, David A.5, Author
Yang, Jin1, Author
Wang, Xingli2, Author
Pachfule, Pradip1, Author
Brückner, Sven2, Author
Jeon, Hyosang4, Author           
Haase, Felix4, Author           
Tsang, Sze-Chun3, Author
Rettenmaier, Clara4, Author           
Chan, Karen3, Author
Roldan Cuenya, Beatriz4, Author           
Thomas, Arne1, Author
Strasser, Peter2, Author
Affiliations:
1Department of Chemistry, Division of Functional Materials, Technical University Berlin, Berlin 10623, Germany, ou_persistent22              
2Department of Chemistry, Chemical Engineering Division, Technical University Berlin, Berlin 10623, Germany, ou_persistent22              
3CatTheory Center, Department of Physics, Technical University of Denmark, 2800 Kongens Lyngby, Denmark, ou_persistent22              
4Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
5Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, USA, ou_persistent22              

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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 electro-reduction to CO, and the single-site Ni-Nx motif is believed as 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.

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Language(s): eng - English
 Dates: 2022-01-282021-10-302022-01-312022-01-312022-04-04
 Publication Status: Issued
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.202114707
 Degree: -

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Title: Angewandte Chemie International Edition
  Abbreviation : Angew. Chem., Int. Ed.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 9 Volume / Issue: 61 (15) Sequence Number: e202114707 Start / End Page: - Identifier: ISSN: 1433-7851
CoNE: https://pure.mpg.de/cone/journals/resource/1433-7851