2026-04-13T20:55:16Zhttps://recercat.cat/oai/request
oai:recercat.cat:2072/4505332024-12-20T20:56:03Zcom_2072_300912com_2072_4427col_2072_301309
RECERCAT author Ismail, Ahmed Mohsen author Samu, Gergely F. author Nguyën, Huu Chuong author Csapó, Edit author López, Núria author Janáky, Csaba 2021-08-23T07:49:54Z2024-04-23T11:06:42Z 2021-08-23T07:49:54Z2024-04-23T11:06:42Z 2020-04-14 http://hdl.handle.net/2072/450533 https://doi.org/10.1021/acscatal.0c00749 The electrochemical conversion of carbon dioxide (CO2) to high-value chemicals is an attractive approach to create an artificial carbon cycle. Tuning the activity and product selectivity while maintaining long-term stability, however, remains a significant challenge. Here, we study a series of Au–Pb bimetallic electrocatalysts with different Au/Pb interfaces, generating carbon monoxide (CO), formic acid (HCOOH), and methane (CH4) as CO2 reduction products. The formation of CH4 is significant because it has only been observed on very few Cu-free electrodes. The maximum CH4 formation rate of 0.33 mA cm–2 was achieved when the most Au/Pb interfaces were present. In situ Raman spectroelectrochemical studies confirmed the stability of the Pb native substoichiometric oxide under the reduction conditions on the Au–Pb catalyst, which seems to be a major contributor to CH4 formation. Density functional theory simulations showed that without Au, the reaction would get stuck on the COOH intermediate, and without O, the reaction would not evolve further than the CHOH intermediate. In addition, they confirmed that the Au/Pb bimetallic interface (together with the subsurface oxygen in the model) possesses a moderate binding strength for the key intermediates, which is indeed necessary for the CH4 pathway. Overall, this study demonstrates how bimetallic nanoparticles can be employed to overcome scaling relations in the CO2 reduction reaction. eng L'accés als continguts d'aquest document queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons:http://creativecommons.org/licenses/by-nc-nd/4.0/ Au/Pb Interface Allows the Methane Formation Pathway in Carbon Dioxide Electroreduction info:eu-repo/semantics/article info:eu-repo/semantics/acceptedVersion URL https://recercat.cat/bitstream/2072/450533/4/ismail_acs_cat_2020.pdf File MD5 4306ef0ad1c6ae69416f6ecb0874bc89 2392577 application/pdf ismail_acs_cat_2020.pdf URL https://recercat.cat/bitstream/2072/450533/5/ismail_acs_cat_2020.pdf.txt File MD5 fc3fc86a181d41ac2c5a60e62ecedeac 54115 text/plain ismail_acs_cat_2020.pdf.txt