The presence and role of the intermediary CO reservoir in heterogeneous electroreduction of CO 2 .

Autor: Louisia S; Department of Chemistry, University of California, Berkeley, CA 94720.; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720., Kim D; Department of Chemistry, University of California, Berkeley, CA 94720.; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720.; Department of Materials Science and Engineering, University of California, Berkeley, CA 94720., Li Y; Department of Chemistry, University of California, Berkeley, CA 94720.; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720., Gao M; Department of Materials Science and Engineering, University of California, Berkeley, CA 94720., Yu S; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720.; Department of Materials Science and Engineering, University of California, Berkeley, CA 94720., Roh I; Department of Chemistry, University of California, Berkeley, CA 94720.; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720., Yang P; Department of Chemistry, University of California, Berkeley, CA 94720.; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720.; Department of Materials Science and Engineering, University of California, Berkeley, CA 94720.; Kavli Energy NanoScience Institute, Berkeley, CA 94720.
Jazyk: angličtina
Zdroj: Proceedings of the National Academy of Sciences of the United States of America [Proc Natl Acad Sci U S A] 2022 May 03; Vol. 119 (18), pp. e2201922119. Date of Electronic Publication: 2022 Apr 29.
DOI: 10.1073/pnas.2201922119
Abstrakt: SignificanceThe electroconversion of CO 2 to value-added products is a promising path to sustainable fuels and chemicals. However, the microenvironment that is created during CO 2 electroreduction near the surface of heterogeneous Cu electrocatalysts remains unknown. Its understanding can lead to the development of ways to improve activity and selectivity toward multicarbon products. This work introduces a method called on-stream substitution of reactant isotope that provides quantitative information of the CO intermediate species present on Cu surfaces during electrolysis. An intermediary CO reservoir that contains more CO molecules than typically expected in a surface adsorbed configuration was identified. Its size was shown to be a factor closely associated with the formation of multicarbon products.
Databáze: MEDLINE