dc.contributor.author | Iyengar, Pranit | |
dc.contributor.author | Kolb, Manuel J. | |
dc.contributor.author | Pankhurst, James R. | |
dc.contributor.author | Calle Vallejo, Federico | |
dc.contributor.author | Buonsanti, Raffaella | |
dc.date.accessioned | 2023-03-21T18:45:10Z | |
dc.date.available | 2023-03-21T18:45:10Z | |
dc.date.issued | 2021-04-07 | |
dc.identifier.citation | ACS Catalysis 11(8) : 4456-4463 (2021) | es_ES |
dc.identifier.issn | 2155-5435 | |
dc.identifier.uri | http://hdl.handle.net/10810/60437 | |
dc.description.abstract | Despite being desirable high-value products of the electrochemical CO2 reduction reaction (CO2RR), alcohols are still obtained with lower selectivity compared to hydrocarbons and the reaction pathways leading to their formation are still under debate. In this joint experimental-computational work, we exploit structural sensitivity effects to elucidate the ethanol-producing active sites on Cu-Ag CO2RR tandem catalysts. Specifically, methane-selective Cu nano-octahedra (Cuoh), enclosed by (111) facets, and ethylene-selective Cu nano-cubes (Cucub), enclosed by (100) facets, are mixed with CO-selective Ag nanospheres (Agsph) to form Cuoh-Ag and Cucub-Ag bimetallic catalysts. Ethanol is selectively enhanced via the *CHx-*CO coupling pathway at the terraces of Cuoh-Ag in the CO-enriched environment generated by the Agsph . Conversely, on Cucub-Ag ethanol is selectively produced via the same pathway at the edges and corners of Cucub while ethylene continues to be produced at the terraces. Such facet dependence explains the higher ethanol-to-ethylene ratio on the Cuoh-Ag. These findings illustrate how tandem catalysis and structure-sensitive effects can be combined to obtain notable changes in the selectivity of electrochemical reactions. | es_ES |
dc.description.sponsorship | This work was financially supported by Gaznat S.A. J.R.P. acknowledges the H2020 Marie Curie Individual Fellowship grant SURFCAT with agreement number 837378. This publication was created as part of NCCR Catalysis, a National Centre of Competence in Research funded by the Swiss National Science Foundation. The theoretical effort was supported by Spanish MICIUN’s RTI2018-095460-B-I00, Ramón y Cajal RYC-2015-18996, and María de Maeztu MDM-2017-0767 grants and partly by Generalitat de Catalunya via 2017SGR13, XRQTC grants. M.J.K. and F.C.-V. are thankful to Red Española de Supercomputación (RES) for supercomputing time at SCAYLE (projects QS-2019-3-0018, QS-2019-2-0023, and QCM-2019-1-0034). The use of supercomputing facilities at SURFsara was sponsored by NWO Physical Sciences. | es_ES |
dc.language.iso | eng | es_ES |
dc.publisher | ACS | es_ES |
dc.relation | info:eu-repo/grantAgreement/EC/H2020/837378 | es_ES |
dc.relation | info:eu-repo/grantAgreement/MICIU/RTI2018-095460-B-I00 | es_ES |
dc.rights | info:eu-repo/semantics/openAccess | es_ES |
dc.subject | facet-dependent selectivity | es_ES |
dc.subject | CO2 electroreduction | es_ES |
dc.subject | ethanol | es_ES |
dc.subject | Cu−Ag tandem catalysts | es_ES |
dc.title | Elucidating the Facet-dependent Selectivity for CO2 Electroreduction to Ethanol of Cu-Ag Tandem Catalysts | es_ES |
dc.type | info:eu-repo/semantics/article | es_ES |
dc.rights.holder | © 2021 American Chemical Society | es_ES |
dc.relation.publisherversion | https://pubs.acs.org/doi/10.1021/acscatal.1c00420 | es_ES |
dc.identifier.doi | 10.1021/acscatal.1c00420 | |
dc.contributor.funder | European Commission | |
dc.departamentoes | Polímeros y Materiales Avanzados: Física, Química y Tecnología | es_ES |
dc.departamentoeu | Polimero eta Material Aurreratuak: Fisika, Kimika eta Teknologia | es_ES |