Towards understanding the active sites for the ORR in N-doped carbon materials through fine-tuning of nitrogen functionalities: an experimental and computational approach
Empreu sempre aquest identificador per citar o enllaçar aquest ítem
http://hdl.handle.net/10045/99193
Títol: | Towards understanding the active sites for the ORR in N-doped carbon materials through fine-tuning of nitrogen functionalities: an experimental and computational approach |
---|---|
Autors: | Quílez-Bermejo, Javier | Melle-Franco, Manuel | San-Fabián, Emilio | Morallon, Emilia | Cazorla-Amorós, Diego |
Grups d'investigació o GITE: | Materiales Carbonosos y Medio Ambiente | Química Cuántica | Electrocatálisis y Electroquímica de Polímeros |
Centre, Departament o Servei: | Universidad de Alicante. Departamento de Química Inorgánica | Universidad de Alicante. Departamento de Química Física | Universidad de Alicante. Instituto Universitario de Materiales |
Paraules clau: | N-doped carbon materials | Oxygen reduction reaction | Nitrogen functionalities |
Àrees de coneixement: | Química Inorgánica | Química Física |
Data de publicació: | 27-de setembre-2019 |
Editor: | American Chemical Society |
Citació bibliogràfica: | Journal of Materials Chemistry A. 2019, 7: 24239-24250. doi:10.1039/C9TA07932G |
Resum: | The design of advanced N-doped carbon materials towards oxygen reduction reaction (ORR) catalysis is only possible if the nature of the active sites is fully understood. There is an important piece of research seeking to overcome this challenge through experimental or theoretical results. However, the combination of both approaches is necessary to deepen the knowledge about this subject. This work presents excellent agreement between experimental results and computational models, which provides evidence of the nature of the most active sites in N-doped carbon materials. N-doped carbon materials have been experimentally obtained through double stage treatment of polyaniline in distinct atmospheres (both oxygen-containing and inert atmospheres) at different temperatures (800–1200 °C). According to temperature programmed desorption (TPD), Raman spectroscopy, N2-adsorption isotherms at −196 °C and X-ray photoelectron spectroscopy (XPS), this synthesis method results in the selective formation of nitrogen species, without significant changes in structural order or porosity. ORR catalytic tests evidence the highly efficient catalysis, with platinum-like performance in terms of the current density and onset potential, of N-doped carbon materials selectively containing graphitic-type nitrogen species. Computational chemistry, through DFT calculations, shows that edge-type graphitic nitrogen is more effective towards ORR catalysis than pyridinic, pyrrolic, pyridonic, oxidized and basal-type graphitic nitrogen species. |
Patrocinadors: | The authors thank Ministerio de Ciencia, Innovación y Universidades and FEDER for financial support (Project RTI2018-095291-B-I00, ENE2017-90932-REDT and FIS2015-64222-C2-2-P). MMF acknowledges support from the Portuguese Foundation for Science and Technology (FCT), under the projects IF/00894/2015, and FCT Ref. UID/CTM/50011/2019 for CICECO - Aveiro Institute of Materials. |
URI: | http://hdl.handle.net/10045/99193 |
ISSN: | 2050-7488 (Print) | 2050-7496 (Online) |
DOI: | 10.1039/C9TA07932G |
Idioma: | eng |
Tipus: | info:eu-repo/semantics/article |
Drets: | © The Royal Society of Chemistry 2019 |
Revisió científica: | si |
Versió de l'editor: | https://doi.org/10.1039/C9TA07932G |
Apareix a la col·lecció: | INV - QC - Artículos de Revistas INV - GEPE - Artículos de Revistas INV - MCMA - Artículos de Revistas |
Arxius per aquest ítem:
Arxiu | Descripció | Tamany | Format | |
---|---|---|---|---|
2019_Quilez-Bermejo_etal_JMaterChemA_final.pdf | Versión final (acceso restringido) | 1,75 MB | Adobe PDF | Obrir Sol·licitar una còpia |
2019_Quilez-Bermejo_etal_JMaterChemA_preprint.pdf | Preprint (acceso abierto) | 1,01 MB | Adobe PDF | Obrir Vista prèvia |
Tots els documents dipositats a RUA estan protegits per drets d'autors. Alguns drets reservats.