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Molybdenum-modified zeolite is the benchmark catalyst reported to date as an effective bi-functional catalyst for methane direct conversion to aromatics and hydrogen without oxygen participation. However, active molybdenum carbide (MoCx) should be first formed at the cost of partial methane during methane dehydroaromatization (MDA). Herein, we reported a method to in situ form molybdenum-based species which were highly dispersed on the ZSM-5 zeolite. During this process, structure-directing agent (SDA) in the zeolite directly reduced molybdenum precursor during calcination in inert atmosphere. The resultant catalyst showed excellent catalytic performance in the MDA reaction. Furthermore, when the active MoCx species were confined in the zeolite, initial activity retained and the catalyst lifetime prolonged over a period of 500 min. [ABSTRACT FROM AUTHOR]