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<p>Photocatalytic CO<sub>2</sub> reduction using H<sub>2</sub>O as the electron donor offers a sustainable pathway for carbon–neutral fuel synthesis; however, its efficiency is limited by sluggish charge separation and insufficient CO<sub>2</sub> activation. Herein, we develop a ruthenium-decorated, fluorine-doped TiO<sub>2</sub> photocatalyst (Ru/F-TiO<sub>2</sub>) that overcomes these limitations through spatially directed charge modulation and cooperative electronic engineering. Fluorine doping introduces oxygen vacancies that narrow the bandgap and form surface Ti‒F bonds, suppressing charge recombination. Simultaneously, Ru nanoparticles serve as efficient CO<sub>2</sub> adsorption and activation centers while introducing additional surface defects that further strengthen CO<sub>2</sub> binding. The strong coupling between Ru and semiconductor forms a Schottky junction, establishing a strong built-in electric field that promotes directional electron migration toward Ru sites and hole accumulation on F-TiO<sub>2</sub>. Consequently, Ru/F-TiO<sub>2</sub> exhibits outstanding activity and durability, delivering CO and CH<sub>4</sub> production rates of 124.8 and 19.8&#xa0;μmol/(g·h), respectively. In situ diffuse reflectance infrared Fourier-transform spectroscopy analysis reveals key proton-coupled, multi-electron intermediates, elucidating the reaction pathway. This study demonstrates that the synergistic integration of non-metal doping and metal cocatalyst engineering provides a powerful strategy to regulate charge dynamics and boost solar-driven CO<sub>2</sub> conversion.</p>

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Engineering Fluorine Doping and Ru–Schottky Interfaces in TiO2 for Efficient Photocatalytic CO2 Reduction with H2O

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月15日

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  • Sichun Ling,
  • Ke Tang,
  • Yafei Zheng,
  • Bo Su,
  • Xiahui Lin,
  • Xue Feng Lu,
  • Yidong Hou,
  • Zhengxin Ding,
  • Sibo Wang

摘要

Photocatalytic CO2 reduction using H2O as the electron donor offers a sustainable pathway for carbon–neutral fuel synthesis; however, its efficiency is limited by sluggish charge separation and insufficient CO2 activation. Herein, we develop a ruthenium-decorated, fluorine-doped TiO2 photocatalyst (Ru/F-TiO2) that overcomes these limitations through spatially directed charge modulation and cooperative electronic engineering. Fluorine doping introduces oxygen vacancies that narrow the bandgap and form surface Ti‒F bonds, suppressing charge recombination. Simultaneously, Ru nanoparticles serve as efficient CO2 adsorption and activation centers while introducing additional surface defects that further strengthen CO2 binding. The strong coupling between Ru and semiconductor forms a Schottky junction, establishing a strong built-in electric field that promotes directional electron migration toward Ru sites and hole accumulation on F-TiO2. Consequently, Ru/F-TiO2 exhibits outstanding activity and durability, delivering CO and CH4 production rates of 124.8 and 19.8 μmol/(g·h), respectively. In situ diffuse reflectance infrared Fourier-transform spectroscopy analysis reveals key proton-coupled, multi-electron intermediates, elucidating the reaction pathway. This study demonstrates that the synergistic integration of non-metal doping and metal cocatalyst engineering provides a powerful strategy to regulate charge dynamics and boost solar-driven CO2 conversion.