Catalytic reduction of CO2 with hydrogen-rich small molecules (e.g., H2, C3H8, and CH4) provides a promising route to valuable chemicals and fuels. However, achieving high catalytic efficiency requires balancing the effective activation of CO2 and hydrogen-rich small molecules with the precise control of dual-site uniformity to ensure cooperative activity. Herein, we propose a high-throughput screening strategy for ternary compounds based on descriptors of structural uniformity, coordination number, and phase stability. The screening identifies three wurtzite-derived crystals, namely ZnGeN2, BeSiN2, and ZnSiN2, with uniform dual frustrated Lewis pairs (FLPs) on their (100) surfaces that are thermally stable up to 873 K. Among them, only the ZnGeN2(100) surface can selectively activate reactants, with Zn···N FLPs favoring CO2 adsorption and Ge···N FLPs activating hydrogen-rich small molecules, due to their intrinsic Lewis acid-base character. Importantly, kinetic Monte Carlo simulations show that the uniform distribution of Zn···N and Ge···N FLPs on ZnGeN2(100) enables efficient pathways, with CO2 consumption rates of 19.67, 1.23, and 2.69 s-1 in the reactions with H2, C3H8, and CH4, respectively. Moreover, the dual FLP remains highly active in CO2 hydrogenation under stoichiometric ratio, CO2-rich, and CO2-lean conditions, ensuring practical reliability.
Yu et al. (Sun,) studied this question.