沸石
甲醇
催化作用
化学
甲烷
产量(工程)
无机化学
氧气
核化学
材料科学
有机化学
冶金
作者
Tássia Caroline Passos Pereira,Joana Vieira,Catarina Cunha,Stefanie C.M. Mizuno,Yasmin Oliveira Carvalho,Thiago Faheina,Monize Picinini,Asdrubal L. Blanco,Ana Cristina Mora Tello,Ernesto A. Urquieta‐González,Alejandro López‐Castillo,Alice Medeiros Lima,João Batista Oliveira dos Santos,J.M.C. Bueno
标识
DOI:10.1016/j.apcatb.2023.123370
摘要
Strong oxidants have been reported to be required in the catalytic oxidation of CH4 to methanol in cyclic processes employing CuO-zeolites. Here, using Cu-exchanged zeolite omega (Cu-MAZ), it was demonstrated that O2 could be replaced by CO2, enabling the development of a new process. CuO-MAZ thermally treated in Ar, O2, or CO2 was investigated using in situ DRS-UV-Vis analysis and spectra calculated using density functional theory. The active species were characterized at different temperatures of reaction with CH4. The species of the type Zn-[CuxOy]n+ and main species Z-[CuOH-HOCu]2+-Z were formed on Cu-MAZ. After the reaction with CH4, the Cu+ formed from Zn-CuxOy could be reoxidized with CO2, while the Cu+ formed from Z-CuOH-HOCu-Z was only reoxidized with H2O, and not with CO2. After reoxidation with H2O, the activity of the material was fully restored by thermal treatment in O2 or CO2. The highest CH3OH yield was achieved using CO2.
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