摘要
Cu aggregation has been a significant obstacle to promoting the catalytic performance of methanol dehydrogenation for the production of high hydrogen storage chemical methyl formate (MF). Catalysts composed of Cu with different loading ( x = 5, 10, 15, 20 wt%) supported on dealuminated mesoporous Y zeolite (mY-deAl) had been prepared by mechanical grinding method and used in methanol dehydrogenation for MF. 10Cu/mY-deAl with appropriate Cu loading exhibited the largest MF yield of 31.9%, which was approximately 30 times higher than that of Cu/mY of 1.0% under 280 °C and 0.2 MPa. The excellent behavior was proved to be attributed to the development of amounts of mesoporous allowing the Cu particle enter into as well as the formation of Al vacancies anchoring optimal amount of Cu, induced by the dealumination of Y. Furthermore, the closely linear relationships between Cu dispersion and TOF Cu , along with that between active Cu 0 concentration and MF selectivity were revealed. The less Cu loading could not provide enough active sites for the conversion of methanol (22.0%) even though having the best dispersion, while the excessive Cu loading would result in Cu aggregation in the mesopores deriving from the limit of Al vacancies. This contribution innovatively provided a kind of Cu supported Y catalyst and clearly elucidated the promotion mechanism of catalytic performance driven by the synergy of Al vacancies and mesopores in methanol dehydrogenation to MF.
危险品化学品经营许可证(带存储)