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 dx2–y2 and dz2 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.