Uniform and Stable Dual Frustrated Lewis Pairs Enabling Highly Efficient Conversion of CO ₂ With Hydrogen‐rich Molecules

Abstract

ABSTRACT Catalytic reduction of CO 2 with hydrogen‐rich small molecules (e.g., H 2 , C 3 H 8 , and CH 4 ) provides a promising route to valuable chemicals and fuels. However, achieving high catalytic efficiency requires balancing the effective activation of CO 2 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 ZnGeN 2 , BeSiN 2 , and ZnSiN 2 , with uniform dual frustrated Lewis pairs (FLPs) on their (100) surfaces that are thermally stable up to 873 K. Among them, only the ZnGeN 2 (100) surface can selectively activate reactants, with Zn···N FLPs favoring CO 2 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 ZnGeN 2 (100) enables efficient pathways, with CO 2 consumption rates of 19.67, 1.23, and 2.69 s −1 in the reactions with H 2 , C 3 H 8 , and CH 4 , respectively. Moreover, the dual FLP remains highly active in CO 2 hydrogenation under stoichiometric ratio, CO 2 ‐rich, and CO 2 ‐lean conditions, ensuring practical reliability.