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<p>Electrocatalytic reduction of CO<sub>2</sub> to fuels and chemicals represents a promising pathway for CO<sub>2</sub> utilization and energy conversion. However, metal-based catalysts often suffer from diminished selectivity in the direct reduction of CO<sub>2</sub> to acetate due to suboptimal intermediate adsorption energy imposed by the linear scaling relationship of <i>d</i>-band theory. We describe a deposition-etching strategy that tunes the <i>sp</i><sup>2</sup>/<i>sp</i><sup>3</sup> hybridization of carbon in diamond to tune the adsorption equilibrium of intermediates for CO<sub>2</sub> reduction to acetate, which circumvents the constraints of the d-band electrons. This metal-free catalyst achieves a Faradaic efficiency of 62.7% for CO<sub>2</sub>-to-acetate conversion and demonstrated 100 hours durability. Mechanistic studies reveal that introducing <i>sp</i><sup>2</sup>-carbons into the <i>sp</i><sup>3</sup>-carbon matrix can control the adsorption energies of *CO<sub>2</sub> and *CO. The <i>sp</i><sup>2</sup>/<i>sp</i><sup>3</sup>-carbon active sites facilitate the formation of the *CHO intermediate, which is asymmetrically coupled with the *CO<sub>L</sub> to generate acetate.</p>

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Selective CO2 reduction to acetate via controlled sp2/sp3 carbon hybridization

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月25日

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  • Chujun Wang,
  • Gong Zhang,
  • Ran Luo,
  • Yixian Wang,
  • Xiao Ma,
  • Mengmeng Zhang,
  • Xin Chang,
  • Zhi-Jian Zhao,
  • Tuo Wang,
  • Jinlong Gong

摘要

Electrocatalytic reduction of CO2 to fuels and chemicals represents a promising pathway for CO2 utilization and energy conversion. However, metal-based catalysts often suffer from diminished selectivity in the direct reduction of CO2 to acetate due to suboptimal intermediate adsorption energy imposed by the linear scaling relationship of d-band theory. We describe a deposition-etching strategy that tunes the sp2/sp3 hybridization of carbon in diamond to tune the adsorption equilibrium of intermediates for CO2 reduction to acetate, which circumvents the constraints of the d-band electrons. This metal-free catalyst achieves a Faradaic efficiency of 62.7% for CO2-to-acetate conversion and demonstrated 100 hours durability. Mechanistic studies reveal that introducing sp2-carbons into the sp3-carbon matrix can control the adsorption energies of *CO2 and *CO. The sp2/sp3-carbon active sites facilitate the formation of the *CHO intermediate, which is asymmetrically coupled with the *COL to generate acetate.