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<p>Oxide-derived copper (OD-Cu) is a promising catalyst for the efficient production of C<sub>2+</sub> products in the electrocatalytic CO<sub>2</sub> reduction reaction. However, the reconstruction processes for the formation of OD-Cu are poorly understood, and the effects of catalyst precursors on performance are not yet clear, which hinder the rational construction of efficient catalysts for the production of C<sub>2+</sub> products. In this work, we propose a strategy of “framework-dissolution” to introduce inert elements to construct different framework structures for Cu–O geometrical coordination modulation. <i>In situ</i> X-ray diffraction and Raman characterizations reveal the effect of different Cu–O geometric coordination on the OD-Cu reconstruction process and the regulation mechanism of the crystal facets. The results demonstrate that OD-Cu exhibits different (200)/(111) facet ratios, with the OD-Cu<sub>t</sub> (200) facet dominating. The catalytic performance of OD-Cu<sub>t</sub> dominated by Cu (200) reaches 75.1% Faradaic efficiency (FE<sub>C2+</sub>) with a partial current density of −187.8 mA cm<sup>−2</sup>. Theoretical calculations indicate that the OD-Cu<sub>t</sub> derived from tetrahedra Cu–O geometric coordination is dominated by the (200) facet, which is favorable to promote the production of C<sub>2+</sub> in CO<sub>2</sub>RR. This work not only fundamentally reveals the structural transformation of electrocatalysts with different Cu–O geometric coordination during the reaction process, but also contributes to the rational design of high-efficiency and low-cost catalysts.</p>

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Cu–O geometric coordination induced facet evolution of derived Cu catalysts for efficient CO2 electroreduction

  • 期刊论文

  • 发表日期：

    2025年5月27日

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  • Xixi Ren,
  • Jiajun Wang,
  • Han Wu,
  • Jinfeng Zhang,
  • Jing Mao,
  • Zongyuan Wang,
  • Kaihang Sun,
  • Ying Chen,
  • Xuerong Zheng,
  • Xiaopeng Han,
  • Yida Deng,
  • Wenbin Hu

摘要

Oxide-derived copper (OD-Cu) is a promising catalyst for the efficient production of C2+ products in the electrocatalytic CO2 reduction reaction. However, the reconstruction processes for the formation of OD-Cu are poorly understood, and the effects of catalyst precursors on performance are not yet clear, which hinder the rational construction of efficient catalysts for the production of C2+ products. In this work, we propose a strategy of “framework-dissolution” to introduce inert elements to construct different framework structures for Cu–O geometrical coordination modulation. In situ X-ray diffraction and Raman characterizations reveal the effect of different Cu–O geometric coordination on the OD-Cu reconstruction process and the regulation mechanism of the crystal facets. The results demonstrate that OD-Cu exhibits different (200)/(111) facet ratios, with the OD-Cut (200) facet dominating. The catalytic performance of OD-Cut dominated by Cu (200) reaches 75.1% Faradaic efficiency (FEC2+) with a partial current density of −187.8 mA cm−2. Theoretical calculations indicate that the OD-Cut derived from tetrahedra Cu–O geometric coordination is dominated by the (200) facet, which is favorable to promote the production of C2+ in CO2RR. This work not only fundamentally reveals the structural transformation of electrocatalysts with different Cu–O geometric coordination during the reaction process, but also contributes to the rational design of high-efficiency and low-cost catalysts.