On the deactivation of N-doped carbon materials active sites during oxygen reduction reaction
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Título: | On the deactivation of N-doped carbon materials active sites during oxygen reduction reaction |
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Autor/es: | Quílez-Bermejo, Javier | Morallon, Emilia | Cazorla-Amorós, Diego |
Grupo/s de investigación o GITE: | Materiales Carbonosos y Medio Ambiente | Electrocatálisis y Electroquímica de Polímeros |
Centro, Departamento o Servicio: | Universidad de Alicante. Departamento de Química Inorgánica | Universidad de Alicante. Departamento de Química Física | Universidad de Alicante. Instituto Universitario de Materiales |
Palabras clave: | Carbon materials | Nitrogen | Electrocatalysts | Oxygen reduction reaction |
Área/s de conocimiento: | Química Inorgánica | Química Física |
Fecha de publicación: | 28-dic-2021 |
Editor: | Elsevier |
Cita bibliográfica: | Carbon. 2022, 189: 548-560. https://doi.org/10.1016/j.carbon.2021.12.086 |
Resumen: | N-doped carbon materials have been considered one of the most promising options for the replacement of platinum-based electrocatalysts towards the oxygen reduction reaction (ORR). This work provides insights into the deactivation routes of N-doped carbon materials. The changes occurring in the active sites of N-doped carbon catalysts have been analyzed in detail through pre- and post-ORR characterization by XPS of selectively N-doped carbon materials. Moreover, computational modelling was used to deepen into the deactivation mechanism of N-doped carbon materials in the ORR. From XPS and computational modelling, it can be concluded that the deactivation of graphitic-type nitrogen species, during the ORR in both acidic and alkaline environments, occurs through oxidation and tautomerization reactions that result in the formation of N–C–O-type groups. In acidic environment, the reaction kinetics is slower due to the high stability of the ORR intermediates. In alkaline electrolyte, the N–C–O-type groups can be easily formed due to the interaction of graphitic-type N species and the OH− anions from the electrolyte. In this case, the catalytic activity is due to the contribution of both graphitic nitrogen groups and N–C–O species. |
Patrocinador/es: | The authors would like to thank MICINN and FEDER (projects PID2019-105923RB-100 and RTI2018-095291-B-I00) for the financial support. |
URI: | http://hdl.handle.net/10045/120731 |
ISSN: | 0008-6223 (Print) | 1873-3891 (Online) |
DOI: | 10.1016/j.carbon.2021.12.086 |
Idioma: | eng |
Tipo: | info:eu-repo/semantics/article |
Derechos: | © 2022 The Authors. Published by Elsevier Ltd. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). |
Revisión científica: | si |
Versión del editor: | https://doi.org/10.1016/j.carbon.2021.12.086 |
Aparece en las colecciones: | INV - GEPE - Artículos de Revistas INV - MCMA - Artículos de Revistas |
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