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<p>We demonstrate that molecular coordination and photothermal excitation synergistically regulate CO<sub>2</sub> electroreduction selectivity on Cu. Phenanthroline (Phen)–functionalized and laser-treated Cu electrodes were investigated under 0.1&#xa0;M KHCO<sub>3</sub> at various conditions. Phen–Cu exhibited a total hydrocarbon Faradaic efficiency (FE) of 19.2% and a chain-growth probability (α) of 0.333, surpassing bare Cu (9.17%, 0.224). Illumination at 520&#xa0;nm triggered localized photothermal activation, quadrupling the C<sub>3+</sub> hydrocarbon FE (0.076%). The optimum Phen concentration (0.25&#xa0;μM) maximized multicarbon selectivity, while deviations in potential or ionic environment shifted selectivity toward C<sub>1</sub> products. EIS analysis revealed the lowest charge-transfer resistance and highest capacitance for Phen–Cu<sub>520</sub>, indicating accelerated interfacial kinetics. XPS and valence-band spectra confirmed Cu<sup>0</sup>/Cu<sup>+</sup> stabilization, persistent N−Cu coordination, and a VB onset shift associated with stronger electronic coupling. These results reveal that ligand-photothermal synergy creates a nonequilibrium, Cu<sup>0</sup>/Cu<sup>+</sup>-rich interface that promotes CO dimerization and chain growth, providing a new strategy for directing electrochemical Fischer–Tropsch-like chemistry.</p>

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Synergistic ligand–photon interactions for enhanced CO2 electroreduction on Cu-based electrodes

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月21日

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  • Huieun Shim,
  • Gaeun Yun,
  • Yunji Gwon,
  • Sooyeon Bae,
  • Hyeonji Lee,
  • Jaehee Shin,
  • Hyojin Nam,
  • Choong Kyun Rhee,
  • Weixin Huang,
  • Youngku Sohn

摘要

We demonstrate that molecular coordination and photothermal excitation synergistically regulate CO2 electroreduction selectivity on Cu. Phenanthroline (Phen)–functionalized and laser-treated Cu electrodes were investigated under 0.1 M KHCO3 at various conditions. Phen–Cu exhibited a total hydrocarbon Faradaic efficiency (FE) of 19.2% and a chain-growth probability (α) of 0.333, surpassing bare Cu (9.17%, 0.224). Illumination at 520 nm triggered localized photothermal activation, quadrupling the C3+ hydrocarbon FE (0.076%). The optimum Phen concentration (0.25 μM) maximized multicarbon selectivity, while deviations in potential or ionic environment shifted selectivity toward C1 products. EIS analysis revealed the lowest charge-transfer resistance and highest capacitance for Phen–Cu520, indicating accelerated interfacial kinetics. XPS and valence-band spectra confirmed Cu0/Cu+ stabilization, persistent N−Cu coordination, and a VB onset shift associated with stronger electronic coupling. These results reveal that ligand-photothermal synergy creates a nonequilibrium, Cu0/Cu+-rich interface that promotes CO dimerization and chain growth, providing a new strategy for directing electrochemical Fischer–Tropsch-like chemistry.