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

论文摘要：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 pro-duction 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 comprehensive understandings of the crucial functions of surface Lewis acid/base sites in the product distribution of solar-driven CO2 reduction.

论文链接：https://www.sciengine.com/SCC/doi/10.1007/s11426-025-2860-7