Advanced search
Start date
Betweenand
(Reference retrieved automatically from Web of Science through information on FAPESP grant and its corresponding number as mentioned in the publication by the authors.)

Insights into the alloy-support synergistic effects for the CO2 hydrogenation towards methanol on oxide-supported Ni5Ga3 catalysts: An experimental and DFT study

Full text
Author(s):
Rasteiro, Leticia F. [1] ; De Sousa, Rafael A. [1] ; Vieira, Luiz H. [1, 2] ; Ocampo-Restrepo, Vivianne K. [1] ; Verga, Lucas G. [1] ; Assaf, Jose M. [2] ; Da Silva, Juarez L. F. [1] ; Assaf, Elisabete M. [1]
Total Authors: 8
Affiliation:
[1] Univ Sao Paulo, Sao Carlos Inst Chem, Av Trabalhador Sao Carlense 400, BR-13560970 Sao Carlos, SP - Brazil
[2] Univ Fed Sao Carlos, Chem Engn Dept, Rod W Luiz, Km 235, BR-13565905 Sao Carlos, SP - Brazil
Total Affiliations: 2
Document type: Journal article
Source: APPLIED CATALYSIS B-ENVIRONMENTAL; v. 302, MAR 2022.
Web of Science Citations: 0
Abstract

Supported Ni-Ga alloys have emerged as potential catalyst to mitigate CO2 emissions by its conversion into methanol at mild conditions, however, its performance depends on the optimization of the alloy-support effects, which is unclear up to now. Herein, we investigate the influence of alloy-support synergy in the catalytic performance of Ni5Ga3 supported on SiO2, CeO2, and ZrO2, by combining in-depth structural, chemical and spectroscopic characterization and density functional theory (DFT) calculations. In situ DRIFTS confirmed further hydrogenation of key reaction intermediates in Ni5Ga3/ZrO2 surface, while weak CO2 adsorption in Ni5Ga3/SiO2 avoided intermediate stabilization on the surface and, strong interaction with Ni5Ga3/CeO2 poisoned interface active sites. Additionally, the relative energies of reactants and key intermediates in the three distinct regions of the catalyst (support surface, alloy surface, and alloy-support interface), calculated through DFT, allowed us to propose a reaction mechanism for the most promising catalyst, Ni5Ga3/ZrO2. (AU)

FAPESP's process: 17/11631-2 - Computational material science and chemistry
Grantee:Juarez Lopes Ferreira da Silva
Support Opportunities: Research Grants - Research Centers in Engineering Program
FAPESP's process: 15/06246-7 - Biorefinery concept applied to biological wastewater treatment plants: environmental pollution control coupled with material and energy recovery
Grantee:Marcelo Zaiat
Support Opportunities: Research Projects - Thematic Grants
FAPESP's process: 19/05561-7 - A Multiscale Framework Applied to the Investigation of CO2 Reduction on Metallic Nanoparticles: The Role of Size and Adsorbate Coverage Effects
Grantee:Lucas Garcia Verga
Support Opportunities: Scholarships in Brazil - Post-Doctorate
FAPESP's process: 18/21401-7 - Multi-User Equipment approved in grant 2017/11631-2: cluster computational de alto desempenho - ENIAC
Grantee:Juarez Lopes Ferreira da Silva
Support Opportunities: Multi-user Equipment Program
FAPESP's process: 18/12021-6 - Partial oxidation of methane to methanol catalyzed by single-atom noble metal (Rh, Pd or Pt) supported on doped mesoporous CeO2 (Ce1-xMxO2, M = Zr, Sn or La)
Grantee:Luiz Henrique Vieira
Support Opportunities: Scholarships in Brazil - Post-Doctorate
FAPESP's process: 14/50279-4 - Brasil Research Centre for Gas Innovation
Grantee:Julio Romano Meneghini
Support Opportunities: Research Grants - Research Centers in Engineering Program
FAPESP's process: 17/22671-5 - Ga-Ni nanoparticles supported on porous silica for methanol synthesis from CO2 at low pressures
Grantee:Letícia Fernanda Rasteiro
Support Opportunities: Scholarships in Brazil - Doctorate
FAPESP's process: 19/22260-0 - Sub-monolayer control of the growth of ZrO2 films over ordered mesoporous silica supports and interface tailoring of Ni-Ga catalysts by atomic layer deposition (ALD)
Grantee:Letícia Fernanda Rasteiro
Support Opportunities: Scholarships abroad - Research Internship - Doctorate