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<p>The electrochemical conversion of CO<sub>2</sub> into multi-carbon (C<sub>2+</sub>) products offers a promising route toward sustainable energy and carbon neutrality, but is hindered by inefficient C–C coupling, especially for C<sub>3</sub> products. Here we show a Ni single atom/Cu single cluster catalyst (Ni SAC/Cu SCC) that achieves a total Faradaic efficiency (FE) of 84.1% for C<sub>2+</sub> products (ethanol, ethylene glycol, and acetone) in a flow cell. The FE for acetone (a C<sub>3</sub> product) reaches 48.8%. The high acetone selectivity on Ni SAC/Cu SCC is attributed to the synergistic interplay among in-tandem catalysis, the confinement effect, and in situ-formed Cu<sup>0</sup>/Cu<sup>+</sup> sites. Mechanistically, CO spills over from Ni sites to adjacent Cu sites and is confined within the hierarchical pore structure of the reduced graphene oxide (rGO) support, resulting in high local CO coverage on Cu sites. Concurrently, the in situ-formed Cu<sup>0</sup>/Cu<sup>+</sup> sites enhance adsorption of the key *CO intermediate. Together, this synergy lowers the energy barriers for C–C coupling. This work provides insights into the electrosynthesis of multi-carbon products.</p>

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In-tandem electrocatalysis via Ni single atoms and reconstructed Cu single clusters for CO2-to-acetone reduction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月21日

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  • Tonglin Yang,
  • Fangqi Yang,
  • Haoming Yu,
  • Xuanzhao Lu,
  • Wenlei Zhu

摘要

The electrochemical conversion of CO2 into multi-carbon (C2+) products offers a promising route toward sustainable energy and carbon neutrality, but is hindered by inefficient C–C coupling, especially for C3 products. Here we show a Ni single atom/Cu single cluster catalyst (Ni SAC/Cu SCC) that achieves a total Faradaic efficiency (FE) of 84.1% for C2+ products (ethanol, ethylene glycol, and acetone) in a flow cell. The FE for acetone (a C3 product) reaches 48.8%. The high acetone selectivity on Ni SAC/Cu SCC is attributed to the synergistic interplay among in-tandem catalysis, the confinement effect, and in situ-formed Cu0/Cu+ sites. Mechanistically, CO spills over from Ni sites to adjacent Cu sites and is confined within the hierarchical pore structure of the reduced graphene oxide (rGO) support, resulting in high local CO coverage on Cu sites. Concurrently, the in situ-formed Cu0/Cu+ sites enhance adsorption of the key *CO intermediate. Together, this synergy lowers the energy barriers for C–C coupling. This work provides insights into the electrosynthesis of multi-carbon products.