Atomically dispersed cerium on copper tailors interfacial water structure for efficient CO-to-acetate electroreduction.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 40118841.
- Also identified by DOI 10.1038/s41467-025-58109-6 and PMC identifier 11928625.
- Licence recorded as CC BY-NC-ND.
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Abstract
Electrosynthesis of acetate from carbon monoxide (CO) powered by renewable electricity offers one promising avenue to obtain valuable carbon-based products but undergoes unsatisfied selectivity because of the competing hydrogen evolution reaction. We report here a cerium single atoms (Ce-SAs) modified crystalline-amorphous dual-phase copper (Cu) catalyst, in which Ce SAs reduce the electron density of the dual-phase Cu, lowering the proportion of interfacial K<sup>+</sup> ion hydrated water (K·H<sub>2</sub>O) and thereby decreasing the H<sup>*</sup> coverage on the catalyst surface. Meanwhile, the electron transfer from dual-phase Cu to Ce SAs yields Cu<sup>+</sup> species, which boost the formation of active atop-adsorbed <sup>*</sup>CO (CO<sub>atop</sub>), improving CO<sub>atop</sub>-CO<sub>atop</sub> coupling kinetics. These together lead to the preferential pathway of ketene intermediate (<sup>*</sup>CH<sub>2</sub>-C=O) formation, which then reacts with OH<sup>-</sup> enriched by pulsed electrolysis to generate acetate. Using this catalyst, we achieve a high Faradaic efficiency of 71.3 ± 2.1% toward acetate and a time-averaged acetate current density of 110.6 ± 2.0 mA cm<sup>-2</sup> under a pulsed electrolysis mode. Furthermore, a flow-cell reactor assembled by this catalyst can produce acetate steadily for at least 138 hours with selectivity greater than 60%.