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<p>Lewis acid (LA) and Lewis base (LB) sites on catalyst surfaces play a pivotal role in catalytic reactions. By precisely modulating the type, density, and spatial distribution of these Lewis acid/base sites, catalytic performance indicators such as catalytic activity, selectivity, and stability can be effectively optimized. As a result, they become essential parameters that must be considered in the design and development of high-efficiency catalysts. This study proposes a surface engineering method to accurately control the concentration of surface LA and LB sites in defect-laden In<sub>2</sub>O<sub>3−<i>x</i></sub>(OH)<sub><i>y</i></sub> (denoted as N-<i>n</i>%-IO), establishing three types of LB/LA stoichiometric ratios with different photocatalytic CO<sub>2</sub> hydrogenation performances. It is demonstrated that the LB-rich system (LB/LA &gt; 1) shows suppressed activity. In contrast, the balanced stoichiometric ratio system (LB/LA = 1) attains an optimal methanol yield (179.79 µmol g<sup>−1</sup> h<sup>−1</sup>) and selectivity (43.67%), while the LA-rich system (LB/LA &lt; 1) exhibits the best CO production rate (1913.76 µmol g<sup>−1</sup> h<sup>−1</sup>) and selectivity (94.96%). Systematic experiments disclose that the balanced LB/LA system with adjacent surface frustrated Lewis pairs (SFLPs) can effectively facilitate the adsorption/activation of reactants, stabilize intermediates, and regulate the dynamic behavior of photo-generated carriers. However, the imbalanced LB/LA systems either lack necessary active sites or can only follow an oxygen vacancy-mediated pathway during photocatalytic CO<sub>2</sub> hydrogenation. This work offers a comprehensive understanding of the crucial functions of surface Lewis acid/base sites in the product distribution of solar-driven CO<sub>2</sub> reduction.</p>

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Decoding the stoichiometry of surface Lewis acid/base sites: a pivotal aspect for tailoring selectivity in solar-driven CO2 reduction

  • 期刊论文

  • 发表日期：

    2025年8月26日

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  • Qinhui Guan,
  • Yuhao Guo,
  • Shuting Li,
  • Xingjuan Li,
  • Xiao Li,
  • Xuan Liu,
  • Na Li,
  • Tingjiang Yan

摘要

Lewis acid (LA) and Lewis base (LB) sites on catalyst surfaces play a pivotal role in catalytic reactions. By precisely modulating the type, density, and spatial distribution of these Lewis acid/base sites, catalytic performance indicators such as catalytic activity, selectivity, and stability can be effectively optimized. As a result, they become essential parameters that must be considered in the design and development of high-efficiency catalysts. This study proposes a surface engineering method to accurately control the concentration of surface LA and LB sites in defect-laden In2O3−x(OH)y (denoted as N-n%-IO), establishing three types of LB/LA stoichiometric ratios with different photocatalytic CO2 hydrogenation performances. It is demonstrated that the LB-rich system (LB/LA > 1) shows suppressed activity. In contrast, the balanced stoichiometric ratio system (LB/LA = 1) attains an optimal methanol yield (179.79 µmol g−1 h−1) and selectivity (43.67%), while the LA-rich system (LB/LA < 1) exhibits the best CO production rate (1913.76 µmol g−1 h−1) and selectivity (94.96%). Systematic experiments disclose that the balanced LB/LA system with adjacent surface frustrated Lewis pairs (SFLPs) can effectively facilitate the adsorption/activation of reactants, stabilize intermediates, and regulate the dynamic behavior of photo-generated carriers. However, the imbalanced LB/LA systems either lack necessary active sites or can only follow an oxygen vacancy-mediated pathway during photocatalytic CO2 hydrogenation. This work offers a comprehensive understanding of the crucial functions of surface Lewis acid/base sites in the product distribution of solar-driven CO2 reduction.