Modification of acidity in HZSM-5 zeolite for methane-methanol co-reactionHZSM-5酸改性及其对甲烷甲醇耦合反应的影响

A co-reaction of methane with methanol over zeolite catalysts has emerged as a new approach to the long-standing challenge of methane transformation. However, the effect of catalyst acid properties on the co-reaction has been rarely studied. In this study, a series of HZSM-5 zeolites with comparable diffusion abilities and various acidities were synthesized directly through steaming with 100% water vapor at 693 K. The co-reaction of methane and methanol was subsequently evaluated. Brønsted acidity at 0.262 mmol/g was detected to reach the maximum methane conversion of 5.42% at 673 K, which was also the odd point in the relationship between acid concentration and C4 hydrogen transfer index. Moreover, the influence of methanol feed was investigated over parent and steamed ZSM-5 catalyst, with results showing that excessive acid sites or methanol molecules reduce methane conversion. It is proposed that acid sites adsorbed with methanol molecules construct the methane activation sites. Hence, a proper design of zeolite acidity should be achieved to obtain higher methane conversion in the co-reaction process.