Author, as appears in the article.: Ma, Haibin; Ibanez-Ale, Enric; You, Futian; Lopez, Nuria; Yeo, Boon Siang
Department: Química Física i Inorgànica
URV's Author/s: Lopez Alonso, Nuria
Keywords: Carbon-monoxide Copper Coverag Electroreduction Identification Multicarbon Ph-dependence Reduction Selectivity Total-energy calculations
Abstract: During the electrochemical CO2 reduction reaction (eCO2RR) on copper catalysts, linear-bonded CO (*COL) is commonly regarded as the key intermediate for the CO-CO coupling step, which leads to the formation of multicarbon products. In this work, we unveil the significant role of bridge-bonded *CO (*COB) as an active species. By combining in situ Raman spectroscopy, gas and liquid chromatography, and density functional theory (DFT) simulations, we show that adsorbed *OH domains displace *COL to *COB. The electroreduction of a 12CO+13CO2 cofeed demonstrates that *COB distinctly favors the production of acetate and 1-propanol, while *COL favors ethylene and ethanol formation. This work enhances our understanding of the mechanistic intricacies of eCO(2)RR and suggests new directions for designing operational conditions by modifying the competitive adsorption of surface species, thereby steering the reaction toward specific multicarbon products.
Thematic Areas: Astronomia / física Biochemistry Catalysis Chemistry Chemistry (all) Chemistry (miscellaneous) Chemistry, multidisciplinary Ciência de alimentos Ciências agrárias i Ciências biológicas i Ciências biológicas ii Colloid and surface chemistry Engenharias ii Engenharias iii Engenharias iv Farmacia General chemistry Interdisciplinar Materiais Química
licence for use: https://creativecommons.org/licenses/by/3.0/es/
Author's mail: nuria.lopez@urv.cat
Record's date: 2024-11-23
Papper version: info:eu-repo/semantics/publishedVersion
Papper original source: Journal Of The American Chemical Society. 146 (44): 30183-30193
APA: Ma, Haibin; Ibanez-Ale, Enric; You, Futian; Lopez, Nuria; Yeo, Boon Siang (2024). Electrochemical Formation of C2+ Products Steered by Bridge-Bonded *CO Confined by *OH Domains. Journal Of The American Chemical Society, 146(44), 30183-30193. DOI: 10.1021/jacs.4c08755
Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
Entity: Universitat Rovira i Virgili
Journal publication year: 2024
Publication Type: Journal Publications
Repositori URV