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Investigation of intermediates formation in the CO2 hydrogenation to methanol reaction over Ni5Ga3-ZrO2-SBA-15 materials prepared via ZrO2 atomic layer deposition

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Autor(es):
Rasteiro, Leticia F. ; Assaf, Jose M. ; Assaf, Elisabete M.
Número total de Autores: 3
Tipo de documento: Artigo Científico
Fonte: Applied Surface Science; v. 654, p. 9-pg., 2024-01-23.
Resumo

The production of methanol through CO2 hydrogenation holds great promise for efficient CO2 utilization. The development of catalysts that exclusively favor the formate route is desirable as this enhances methanol selectivity and avoids CO formation. Here, the synthesis of two groups of Ni5Ga3-ZrO2-SBA-15 based materials was studied through the atomic layer deposition (ALD) of ZrO2. The first group was prepared applying ZrO2 ALD over a Ni5Ga3/SBA-15 material and the second group was prepared doing ZrO2 ALD over a mesoporous silica, Santa Barbara Amorphous (SBA-15), followed by impregnation with Ni5Ga3. Some characterization techniques were employed to assess the effectiveness of the ZrO2 ALD on both groups. Interestingly, it was observed that ZrO2 deposition was less effective over the Ni5Ga3/SBA-15 sample compared to its deposition over pure SBA-15, and through XPS analysis was noticed that ZrO2 is probably covering part of the Ni5Ga3 alloys. Furthermore, in situ DRIFTS analysis was performed during reaction conditions and revealed that ZrO2 deposition facilitated the formation of formate and methoxy intermediates in both material groups. The increase in the ZrO2 ALD cycles increased the formate and methoxy bands and decreased CO-related bands. After 6 cycles, only the ZrSBANG_6 catalyst exclusively followed the formate route, as only formate and methoxy bands were present. (AU)

Processo FAPESP: 15/06246-7 - Aplicação do conceito de biorrefinaria a estações de tratamento biológico de águas residuárias: o controle da poluição ambiental aliado à recuperação de matéria e energia
Beneficiário:Marcelo Zaiat
Modalidade de apoio: Auxílio à Pesquisa - Temático
Processo FAPESP: 17/22671-5 - Nanopartículas de Ga-Ni suportados em sílica porosa para a síntese de metanol a partir do CO2 em baixas pressões
Beneficiário:Letícia Fernanda Rasteiro
Modalidade de apoio: Bolsas no Brasil - Doutorado
Processo FAPESP: 18/12021-6 - Oxidação parcial do metano a metanol utilizando catalisadores de metais nobres (Rh, Pd ou Pt) atomicamente dispersos na superfície de CeO2 mesoporosos dopados (Ce1-xMxO2, M=Zr, Sn ou La)
Beneficiário:Luiz Henrique Vieira
Modalidade de apoio: Bolsas no Brasil - Pós-Doutorado
Processo FAPESP: 14/50279-4 - Brasil Research Centre for Gas Innovation
Beneficiário:Julio Romano Meneghini
Modalidade de apoio: Auxílio à Pesquisa - Programa Centros de Pesquisa Aplicada