Uniform and Stable Dual Frustrated Lewis Pairs Enabling Highly Efficient Conversion of CO₂ With Hydrogen-rich...

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.