2026-04-17T17:16:42Zhttps://recercat.cat/oai/request

oai:recercat.cat:2072/4631922025-10-13T09:35:08Zcom_2072_98col_2072_378192

urn:hdl:2072/463192 Engineering the Interfacial Microenvironment via Surface Hydroxylation to Realize the Global Optimization of Electrochemical CO Reduction Han, Xu Zhang, Ting Biset-Peiró, Martí Zhang, Xuan Li, Jian Tang, Weiqiang Tang, PengYi Morante, Joan Ramon Arbiol i Cobos, Jordi ZnO Surficial hydroxyls CO adsorption CO activation Metal-organic frameworks (MOFs) The adsorption and activation of CO on the electrode interface is a prerequisite and key step for electrocatalytic CO reduction reaction (eCO RR). Regulating the interfacial microenvironment to promote the adsorption and activation of CO is thus of great significance to optimize overall conversion efficiency. Herein, a CO-philic hydroxyl coordinated ZnO (ZnO-OH) catalyst is fabricated, for the first time, via a facile MOF-assisted method. In comparison to the commercial ZnO, the as-prepared ZnO-OH exhibits much higher selectivity toward CO at lower applied potential, reaching a Faradaic efficiency of 85% at -0.95 V versus RHE. To the best of our knowledge, such selectivity is one of the best records in ZnO-based catalysts reported till date. Density functional theory calculations reveal that the coordinated surficial -OH groups are not only favorable to interact with CO molecules but also function in synergy to decrease the energy barrier of the rate-determining step and maintain a higher charge density of potential active sites as well as inhibit undesired hydrogen evolution reaction. Our results indicate that engineering the interfacial microenvironment through the introduction of CO-philic groups is a promising way to achieve the global optimization of eCO RR via promoting adsorption and activation of CO. 2022 Article Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-327 Agència de Gestió d'Ajuts Universitaris i de Recerca 2017/SGR-1246 Agencia Estatal de Investigación PID2020-116093RB-C42 Agencia Estatal de Investigación PID2020-116093RB-C43 Ministerio de Ciencia e Innovación SEV-2017-0706 ACS applied materials & interfaces ; Vol. 14, Issue 28 (July 2022), p. 32157-32165 open access Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original. https://creativecommons.org/licenses/by/4.0/