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<p>Confronting the intertwined challenges of climate change and sustainable energy, the advancement of carbon–neutral technologies relying on catalytic carbon dioxide reduction reactions (CO<sub>2</sub>RR) is imperative. While experimental studies have significantly progressed in elucidating catalytic reaction mechanisms, existing theoretical frameworks remain insufficient in deciphering the synergistic regulation mechanisms between crystal facet effects and solvation interactions. This study leverages density functional theory (DFT) calculations to systematically explore the catalytic properties of various copper-based catalyst facets. Moreover, it investigates the regulatory mechanisms of three distinct water molecular microenvironments on the electrochemical CO<sub>2</sub> reduction to methane. Results reveal that although water molecular environments can modulate reaction energy barriers by influencing intermediate adsorption, they cannot disrupt the inherent linear correlations of intermediate binding energies on metallic catalyst surfaces. Synergistic modulation strategies integrating catalyst electronic structure engineering and solvation microenvironment design are essential for optimizing reaction kinetics and product selectivity, providing crucial theoretical guidance for copper-based catalyst design.</p>

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Mechanistic insights into the impact of locally ordered versus disordered aqueous environments on CO2 reduction to methane across copper surfaces

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年7月29日

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  • Zhiguo Xing,
  • Mingzi Sun,
  • Haitao Yu,
  • Xiao Wu,
  • Jiahao Kou,
  • Shipeng Liang,
  • Bolong Huang

摘要

Confronting the intertwined challenges of climate change and sustainable energy, the advancement of carbon–neutral technologies relying on catalytic carbon dioxide reduction reactions (CO2RR) is imperative. While experimental studies have significantly progressed in elucidating catalytic reaction mechanisms, existing theoretical frameworks remain insufficient in deciphering the synergistic regulation mechanisms between crystal facet effects and solvation interactions. This study leverages density functional theory (DFT) calculations to systematically explore the catalytic properties of various copper-based catalyst facets. Moreover, it investigates the regulatory mechanisms of three distinct water molecular microenvironments on the electrochemical CO2 reduction to methane. Results reveal that although water molecular environments can modulate reaction energy barriers by influencing intermediate adsorption, they cannot disrupt the inherent linear correlations of intermediate binding energies on metallic catalyst surfaces. Synergistic modulation strategies integrating catalyst electronic structure engineering and solvation microenvironment design are essential for optimizing reaction kinetics and product selectivity, providing crucial theoretical guidance for copper-based catalyst design.