Efficient Conversion of CO<sub>2</sub> to Ethanol by Utilizing the Topological Surface States of Rare-Earth Cuprates.
basic_science · Level V
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- Record sourced from PubMed, PMID 39908396.
- Also identified by DOI 10.1021/acs.nanolett.4c05719.
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Abstract
The design of high-performance catalysts for the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) remains a significant challenge in advancing CO<sub>2</sub> conversion and storage technologies. In this study, we explored the novel application of topological materials for CO<sub>2</sub>RR, with a focus on the production of high-value C<sub>2+</sub> products. Among 14 lanthanum cuprates, Pr<sub>2</sub>CuO<sub>4</sub> was identified as a promising candidate due to its robust topological surface states (TSS) and potential selectivity for C<sub>2+</sub> products. Electrocatalytic experiments demonstrated excellent and stable selectivity, achieving over 67% ethanol production with a current density of up to 220 mA cm<sup>-2</sup>. Detailed analysis revealed strong interactions between the C p orbital of key intermediates and the Cu d<sub><i>x</i><sup>2</sup>-<i>y</i><sup>2</sup></sub> and d<sub><i>z</i><sup>2</sup></sub> 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.