In situ Raman spectroscopic evidence for oxygen reduction reaction intermediates at platinum single-crystal surfaces
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Título: | In situ Raman spectroscopic evidence for oxygen reduction reaction intermediates at platinum single-crystal surfaces |
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Autor/es: | Dong, Jin-Chao | Zhang, Xia-Guang | Briega-Martos, Valentín | Jin, Xi | Yang, Ji | Chen, Shu | Yang, Zhi-Lin | Wu, De-Yin | Feliu, Juan M. | Williams, Christopher T. | Tian, Zhong-Qun | Li, Jian-Feng |
Grupo/s de investigación o GITE: | Electroquímica de Superficies |
Centro, Departamento o Servicio: | Universidad de Alicante. Departamento de Química Física | Universidad de Alicante. Instituto Universitario de Electroquímica |
Palabras clave: | Electrocatalysis | In situ Raman spectroscopy | Oxygen reduction reaction | Platinum single-crystal surfaces |
Área/s de conocimiento: | Química Física |
Fecha de publicación: | 3-dic-2018 |
Editor: | Springer Nature |
Cita bibliográfica: | Nature Energy. 2019, 4: 60-67. doi:10.1038/s41560-018-0292-z |
Resumen: | Developing an understanding of structure–activity relationships and reaction mechanisms of catalytic processes is critical to the successful design of highly efficient catalysts. As a fundamental reaction in fuel cells, elucidation of the oxygen reduction reaction (ORR) mechanism at Pt(hkl) surfaces has remained a significant challenge for researchers. Here, we employ in situ electrochemical surface-enhanced Raman spectroscopy (SERS) and density functional theory (DFT) calculation techniques to examine the ORR process at Pt(hkl) surfaces. Direct spectroscopic evidence for ORR intermediates indicates that, under acidic conditions, the pathway of ORR at Pt(111) occurs through the formation of HO2*, whereas at Pt(110) and Pt(100) it occurs via the generation of OH*. However, we propose that the pathway of the ORR under alkaline conditions at Pt(hkl) surfaces mainly occurs through the formation of O2−. Notably, these results demonstrate that the SERS technique offers an effective and reliable way for real-time investigation of catalytic processes at atomically flat surfaces not normally amenable to study with Raman spectroscopy. |
Patrocinador/es: | This work was supported by the NSFC (21522508, 21427813, 21521004, 21533006, 21621091 and 21775127), “111” Project (B17027), Natural Science Foundation of Guangdong Province (2016A030308012), the Fundamental Research Funds for the Central Universities (20720180037), and the Thousand Youth Talents Plan of China. Support from MINECO and Generalitat Valenciana (Spain), through projects CTQ2016–76221-P (AEI/FEDER, UE) and PROMETEOII/2014/013, respectively, is greatly acknowledged. V.B.-M. acknowledges MINECO for the award of a pre-doctoral grant (BES-2014–068176, project CTQ2013–44803-P). |
URI: | http://hdl.handle.net/10045/87254 |
ISSN: | 2058-7546 |
DOI: | 10.1038/s41560-018-0292-z |
Idioma: | eng |
Tipo: | info:eu-repo/semantics/article |
Derechos: | © The Author(s), under exclusive licence to Springer Nature Limited 2018 |
Revisión científica: | si |
Versión del editor: | https://doi.org/10.1038/s41560-018-0292-z |
Aparece en las colecciones: | INV - EQSUP - Artículos de Revistas |
Archivos en este ítem:
Archivo | Descripción | Tamaño | Formato | |
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2019_Dong_etal_NatureEnergy_final.pdf | Versión final (acceso restringido) | 2,09 MB | Adobe PDF | Abrir Solicitar una copia |
2019_Dong_etal_NatureEnergy_revised.pdf | Versión revisada (acceso abierto) | 8,44 MB | Adobe PDF | Abrir Vista previa |
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