In Situ Observation of Post‐CO Intermediates to Decode C─C Coupling Pathways in CO_2 Electroreduction

IR (HANDLE) Open Access
  • Sun, Mingxu
    Institute for Frontier Science, State Key Laboratory of Mechanics and Control of Mechanical Structure and Key Laboratory for Intelligent Nano Materials and Devices of the Ministry of Education, Nanjing University of Aeronautics and Astronautics Institute for Materials Chemistry and Engineering (IMCE), Kyushu University Department of Chemistry, Graduate School of Science, Kyushu University
  • Rocabado, David S. Rivera
    Graduate School of Advanced Science and Engineering, Hiroshima University International Research and Education Center, Graduate School of Science, Osaka Metropolitan University Department of Chemistry, Graduate School of Science, Osaka Metropolitan University
  • Cheng, Jiamin
    Research Center for Negative Emissions Technologies (K-NETs), Kyushu University
  • Noguchi, Tomohiro G.
    Institute for Materials Chemistry and Engineering (IMCE), Kyushu University
  • Donoshita, Masaki
    Institute for Materials Chemistry and Engineering (IMCE), Kyushu University
  • Matsuu, Takahiro
    Department of Chemistry, Graduate School of Science, Kyushu University
  • Higashi, Manabu
    Institute for Materials Chemistry and Engineering (IMCE), Kyushu University
  • Fujigaya, Tsuyohiko
    Department of Applied Chemistry, Graduate School of Engineering, Kyushu University Center for Molecular Systems (CMS), Kyushu University International Institute for Carbon‐Neutral Energy Research (WPI‐I^2 CNER), Kyushu University
  • Ishimoto, Takayoshi
    Graduate School of Advanced Science and Engineering, Hiroshima University
  • Yamauchi, Miho
    Institute for Materials Chemistry and Engineering (IMCE), Kyushu University Research Center for Negative Emissions Technologies (K-NETs), Kyushu University International Institute for Carbon‐Neutral Energy Research (WPI‐I^2 CNER), Kyushu University Advanced Institute for Materials Research (WPI-AIMR), Tohoku University

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Description

Electrocatalytic carbon dioxide (CO_2) reduction reaction (CO_2RR) has emerged as a promising strategy for sustainable energy conversion and carbon utilization. Despite intensive research efforts, the understanding of intermediates and pathways leading from CO_2RR to multicarbon (C_<2+>) chemicals remains incomplete. The challenge is to gain insight into the activation of adsorbed CO and the subsequent pathways. Here, we design a specially tailored Cu nanowire array facing a hydrophobic interface as an electrode to highly enhance Raman signals in the in situ environment, allowing sensitive observation of the sequential change of various elusive intermediates during CO_2RR, such as CO, CH_2, CO coexisting with CH_2, CH_2CO, and CH_3. Density functional theory calculations reveal that the C─C coupling during CO_2RR originates from an asymmetric coupling between CH_2 and CO to form CH_2CO, identified as the rate-determining step in the formation of C_<2+> products. These findings deepen the understanding of the C─C coupling processes, which are crucial for advancing catalyst development in electrochemical CO_2 upgrading.

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Details 詳細情報について

  • CRID
    1050585869110503424
  • NII Book ID
    AA0052535X
  • ISSN
    15213773
    14337851
  • HANDLE
    2324/7360333
  • Text Lang
    en
  • Article Type
    journal article
  • Data Source
    • IRDB

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