| Texto completo | |
| Autor(es): |
De Sousa, Rafael A.
;
Ocampo-Restrepo, Vivianne K.
;
Verga, Lucas G.
;
Da Silva, Juarez L. F.
Número total de Autores: 4
|
| Tipo de documento: | Artigo Científico |
| Fonte: | Journal of Chemical Physics; v. 156, n. 21, p. 14-pg., 2022-06-07. |
| Resumo | |
The Ni5Ga3 alloy supported on ZrO2 is a promising catalyst for the reduction of CO2 due to its higher selectivity to methanol at ambient pressure, e.g., activity comparable to industrial catalysts. However, our atomistic understanding of the role of the cooperative effects induced by the Ni5Ga3 alloy formation and its Ni5Ga3/ZrO2 interface in the CO2 reduction is still far from satisfactory. In this work, we tackle these questions by employing density functional theory calculations to investigate the adsorption properties of key CO2 reduction intermediates (CO2, H-2, cis-COOH, trans-COOH, HCOO, CO, HCO, and COH) on Ni-8, Ga-8, Ni5Ga3, (ZrO2)(16), and Ni5Ga3/(ZrO2)(16). We found that Ni containing clusters tended to assume wetting configurations on the (ZrO2)(16) cluster, while the presence of Ga atoms weakens the adsorption energies on the oxide surface. We also observed that CO2 was better activated on the metal-oxide interfaces and on the oxide surface, where it was able to form CO3-like structures. Meanwhile, H-2 activation was only observed on Ni sites, which indicates the importance of distinct adsorption sites that can favor different CO2 reduction steps. Moreover, the formation of the metal-oxide interface showed to be beneficial for the adsorption of COOH isomers and unfavorable for the adsorption of HCOO. Published under an exclusive license by AIP Publishing. (AU) | |
| Processo FAPESP: | 21/07129-5 - Redução de CO2 em superfícies intermetálicas de Cu-Au: efeitos do ordenamento atômico e concentração de adsorvatos |
| Beneficiário: | Lucas Garcia Verga |
| Modalidade de apoio: | Bolsas no Exterior - Estágio de Pesquisa - Pós-Doutorado |
| Processo FAPESP: | 19/05561-7 - Simulações Mutiescala Aplicadas à Redução do CO2 em Nanopartículas Metálicas: Efeitos de Tamanho das Nanopartículas e Concentração de Adsorvatos |
| Beneficiário: | Lucas Garcia Verga |
| Modalidade de apoio: | Bolsas no Brasil - Pós-Doutorado |
| Processo FAPESP: | 18/21401-7 - EMU concedido no processo 2017/11631-2: cluster computacional de alto desempenho - ENIAC |
| Beneficiário: | Juarez Lopes Ferreira da Silva |
| Modalidade de apoio: | Auxílio à Pesquisa - Programa Equipamentos Multiusuários |
| Processo FAPESP: | 17/11631-2 - CINE: desenvolvimento computacional de materiais utilizando simulações atomísticas, meso-escala, multi-física e inteligência artificial para aplicações energéticas |
| Beneficiário: | Juarez Lopes Ferreira da Silva |
| Modalidade de apoio: | Auxílio à Pesquisa - Programa Centros de Pesquisa Aplicada |