Efficient Conversion of CO2 to Ethanol by Utilizing the Topological Surface States of Rare-Earth Cuprates

The design of high-performance catalysts for the CO₂ reduction reaction (CO₂RR) remains a significant challenge in advancing CO₂ conversion and storage technologies. In this study, we explored the novel application of topological materials for CO₂RR, with a focus on the production of high-value C₂₊ products. Among 14 lanthanum cuprates, Pr₂CuO₄ was identified as a promising candidate due to its robust topological surface states (TSS) and potential selectivity for C₂₊ products. Electrocatalytic experiments demonstrated excellent and stable selectivity, achieving over 67% ethanol production with a current density of up to 220 mA cm^-2. Detailed analysis revealed strong interactions between the C p orbital of key intermediates and the Cu d_x²-y² and d_z² orbitals, which are identified as the primary contributors to TSS. These interactions significantly enhanced charge transfer along the desired reaction pathway, indicating that the interplay between the orbitals of key intermediates and TSS-contributing orbitals could be pivotal for developing new paradigms in catalyst design by leveraging topological effects.