Unravelling catalytic activity trends in ceria surfaces toward the oxygen reduction and water oxidation reactions

Autor(es)

Lucchetti, Lanna E. B. ; Autreto, Pedro A. S. ; de Almeida, James M. M. ; Santos, Mauro C. C. ; Siahrostami, Samira

• Tipo de documento: Artigo Científico
• Fonte: REACTION CHEMISTRY & ENGINEERING; v. 8, n. 6, p. 9-pg., 2023-03-03.

Resumo

Improved catalysts are critical for more environmentally friendly, and long-term oxygen electrochemical reactions. Computational catalysis can provide atomic level information that is critical for optimizing the next generation of electrocatalysts. It has been demonstrated that by varying the exposed planes, the catalytic performance of metallic oxides can be tuned. Herein, we investigate the role of CeO2 surface orientations (100), (110), (111), (221), and (331) in enhancing catalytic activity toward various oxygen electrochemical reactions ranging from 4- and 2-electron oxygen reduction reactions (ORR) to 4-, 2- and 1-electron water oxidation reactions (WOR) using density functional theory (DFT) calculations in conjunction with the computational hydrogen electrode. Our results indicate that the CeO2(100) facet is the most promising for 4-electron ORR, with a theoretical limiting potential of 0.52 V. We also show that the presence of oxygen vacancies can enhance the 4-electron ORR activity of the CeO2(110) and CeO2(111) surfaces. Besides, CeO2(100) is selective for the 4-electron WOR while CeO2(110) and CeO2(111) are selective for the 2-electron and 1-electron WOR, respectively. Oxygen vacancies shift all the above three facets towards the 4-electron WOR. This work sheds light on the role of different ceria facets in various oxygen electrochemical reactions which is critical for developing better catalysts. (AU)

• Processo FAPESP: 17/10118-0 - Estudo e aplicação da tecnologia eletroquímica para a análise e a degradação de interferentes endócrinos: materiais, sensores, processos e divulgação científica
• Beneficiário: Marcos Roberto de Vasconcelos Lanza
• Modalidade de apoio: Auxílio à Pesquisa - Temático
• Processo FAPESP: 19/01925-4 - Aplicação de eletrodos de difusão gasosa modificados com materiais avançados na eletrossíntese de peróxido de hidrogênio e posterior degradação de poluentes orgânicos
• Beneficiário: Lanna Emilli Barbosa Lucchetti
• Modalidade de apoio: Bolsas no Brasil - Doutorado Direto