| Texto completo | |
| Autor(es): |
Felicio-Sousa, Priscilla
;
Andriani, Karla F.
;
Da Silva, Juarez L. F.
Número total de Autores: 3
|
| Tipo de documento: | Artigo Científico |
| Fonte: | Physical Chemistry Chemical Physics; v. 23, n. 14, p. 13-pg., 2021-03-04. |
| Resumo | |
Here, we report a theoretical investigation, based on density functional theory calculations, into the role of the occupation d-states on the adsorption properties of CH4, CO, H-2 and CH3OH on 3d 13-atom transition-metal (TM13) clusters (TM = Fe, Co, Ni, Cu). Except for Cu-13, a gradual increase in the occupation of the d-states, i.e., from Fe-13 to Ni-13, increases the magnitude of the adsorption energy almost linearly for the H-2/TM13 and CO/TM13 systems, which can be explained by the enhancement of the sp-d hybridization due to the shift of the d-states towards the highest occupied molecular orbital (HOMO). For Cu-13, the d-states are located well below the HOMO, which reduces the sp-d hybridization, and hence, a smaller adsorption energy is obtained. However, this picture does not hold for CH4/TM13 and CH3OH/TM13, where the adsorption energy has nearly the same value for all TM13 clusters, which can be explained by electrostatic effects such as local polarization of the molecules and nearby TM atoms, and hence, the basic features of physisorption systems. Based on the electron density difference, the polarization effects are slightly larger for systems with empty d-states. (AU) | |
| 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 |
| 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: | 18/11152-0 - Desenvolvimento de catalisadores para conversão direta de metano em metanol: uma investigação ab initio utilizando a da Teoria Funcional da Densidade |
| Beneficiário: | Karla Furtado Andriani |
| Modalidade de apoio: | Bolsas no Brasil - Pós-Doutorado |