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Elucidating electrochemical nitrate and nitrite reduction over atomically-dispersed transition metal sites.
Murphy, Eamonn; Liu, Yuanchao; Matanovic, Ivana; Rüscher, Martina; Huang, Ying; Ly, Alvin; Guo, Shengyuan; Zang, Wenjie; Yan, Xingxu; Martini, Andrea; Timoshenko, Janis; Cuenya, Beatriz Roldán; Zenyuk, Iryna V; Pan, Xiaoqing; Spoerke, Erik D; Atanassov, Plamen.
Afiliação
  • Murphy E; Department of Chemical and Biomolecular Engineering, University of California, Irvine, CA, 92697, USA.
  • Liu Y; Department of Chemical and Biomolecular Engineering, University of California, Irvine, CA, 92697, USA.
  • Matanovic I; Department of Chemical and Biological Engineering, University of New Mexico, Albuquerque, NM, 87131, USA.
  • Rüscher M; Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA.
  • Huang Y; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, 4-6 Faradayweg, Berlin, 14195, Germany.
  • Ly A; Department of Materials Science and Engineering, University of California, Irvine, CA, 92697, USA.
  • Guo S; Department of Materials Science and Engineering, University of California, Irvine, CA, 92697, USA.
  • Zang W; Department of Chemical and Biomolecular Engineering, University of California, Irvine, CA, 92697, USA.
  • Yan X; Department of Materials Science and Engineering, University of California, Irvine, CA, 92697, USA.
  • Martini A; Department of Materials Science and Engineering, University of California, Irvine, CA, 92697, USA.
  • Timoshenko J; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, 4-6 Faradayweg, Berlin, 14195, Germany.
  • Cuenya BR; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, 4-6 Faradayweg, Berlin, 14195, Germany.
  • Zenyuk IV; Department of Interface Science, Fritz Haber Institute of the Max Planck Society, 4-6 Faradayweg, Berlin, 14195, Germany.
  • Pan X; Department of Chemical and Biomolecular Engineering, University of California, Irvine, CA, 92697, USA.
  • Spoerke ED; Department of Materials Science and Engineering, University of California, Irvine, CA, 92697, USA.
  • Atanassov P; Department of Materials Science and Engineering, University of California, Irvine, CA, 92697, USA.
Nat Commun ; 14(1): 4554, 2023 Jul 28.
Article em En | MEDLINE | ID: mdl-37507382
ABSTRACT
Electrocatalytic reduction of waste nitrates (NO3-) enables the synthesis of ammonia (NH3) in a carbon neutral and decentralized manner. Atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts demonstrate a high catalytic activity and uniquely favor mono-nitrogen products. However, the reaction fundamentals remain largely underexplored. Herein, we report a set of 14; 3d-, 4d-, 5d- and f-block M-N-C catalysts. The selectivity and activity of NO3- reduction to NH3 in neutral media, with a specific focus on deciphering the role of the NO2- intermediate in the reaction cascade, reveals strong correlations (R=0.9) between the NO2- reduction activity and NO3- reduction selectivity for NH3. Moreover, theoretical computations reveal the associative/dissociative adsorption pathways for NO2- evolution, over the normal M-N4 sites and their oxo-form (O-M-N4) for oxyphilic metals. This work provides a platform for designing multi-element NO3RR cascades with single-atom sites or their hybridization with extended catalytic surfaces.
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Revista: Nat Commun Assunto da revista: BIOLOGIA / CIENCIA Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Estados Unidos
Texto completo
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PubMed Links
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Revista: Nat Commun Assunto da revista: BIOLOGIA / CIENCIA Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Estados Unidos