Effect of operating parameters on H-2/CO2 conversion to methanol over Cu-Zn oxide supported on ZrO2 polymorph catalysts: Characterization and kinetics

Autor(es)

Marcos, Francielle C. F. ^[1] ; Cavalcanti, Fabio M. ^[1] ; Petrolini, Davi D. ^[2] ; Lin, Lili ^[3] ; Betancourt, Luis E. ^[3] ; Senanayake, Sanjaya D. ^[3] ; Rodriguez, Jose A. ^[3] ; Assaf, Jose M. ^[4] ; Giudici, Reinaldo ^[1] ; Assaf, Elisabete M. ^[2]

Afiliação do(s) autor(es)

^[1] Univ Sao Paulo, Dept Chem Engn, Escola Politecn, Av Prof Luciano Gualberto, T 3, 380, BR-05508010 Sao Paulo, SP - Brazil

^[2] Univ Sao Paulo, Sao Carlos Inst Chem, Av Trabalhador Sao Carlense 400, BR-13560970 Sao Carlos, SP - Brazil

^[3] Brookhaven Natl Lab, Chem Dept, Upton, NY 11973 - USA

^[4] Univ Fed Sao Carlos, Rod W Luiz Km 235, BR-13565905 Sao Carlos, SP - Brazil

• Tipo de documento: Artigo Científico
• Fonte: CHEMICAL ENGINEERING JOURNAL; v. 427, JAN 1 2022.
• Citações Web of Science: 1

Resumo

Kinetic aspects of the operating parameters for the catalytic conversion of H-2/CO2 to methanol over two novel catalysts were evaluated to understand the effect of the polymorphic ZrO2 phase composed of Cu0/+-ZnO sites at the atomic level and its impact on the reaction mechanism. The catalysts were characterized by in situ and ex-situ XRD, N-2 adsorption/desorption isotherms, FRX, TPR, TPD-N2O, in situ XANES, TPD-CO2, and in situ DRIFTS techniques. The influence of different reaction variables such as the GHSV, temperature, pressure, and H-2/CO2 ratio were studied using a fixed bed continuous plug flow reactor. The Cu-ZnO catalyst supported on the tetragonal zirconia polymorph exhibited the highest methanol yield due to the lower activation energy when compared to the catalyst with a greater amount of the monoclinic phase. In addition, the catalysts were reused for 8 cycles of 6 h to evaluate their stability, which can translate into lower costs for large-scale methanol production. The estimation of the kinetic parameters for the Cu-Zn oxide catalysts supported on ZrO2 polymorphs was important to understand the reaction mechanism, as well as to provide useful information for scaling up the process. (AU)

• Processo FAPESP: 19/10980-9 - Acoplamento oxidativo do metano utilizando catalisadores do tipo A2B2O7
• Beneficiário: Davi Domingos Petrolini
• Modalidade de apoio: Bolsas no Brasil - Pós-Doutorado
• Processo FAPESP: 17/08293-8 - Projeto 14: síntese direta de metanol a partir de CO2
• Beneficiário: Francielle Candian Firmino Marcos
• Modalidade de apoio: Bolsas no Brasil - Pós-Doutorado
• Processo FAPESP: 17/11940-5 - Avaliação de catalisadores suportados em nanotubos de carbono e modelagem cinética do processo para a reação de Water-Gas-Shift (WGS)
• Beneficiário: Fábio Machado Cavalcanti
• Modalidade de apoio: Bolsas no Brasil - 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 em Engenharia
• Processo FAPESP: 18/05799-0 - Estudo da superfície de catalisadores de Cu-Ga/ZrO2 para a síntese de metanol
• Beneficiário: Francielle Candian Firmino Marcos
• Modalidade de apoio: Bolsas no Exterior - Estágio de Pesquisa - Pós-Doutorado