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Despite its original discovery over half a century ago over the zeolite ZSM\u20105, the practical application of this process in a CO<jats:sub>2<\/jats:sub>\u2010neutral scenario has faced several obstacles. One prominent challenge has been the intricate mechanistic complexities inherent in the MTH process over the zeolite ZSM\u20105, impeding its widespread adoption. This work takes a significant step forward by providing critical insights that bridge the gap in our understanding of the MTH process. It accomplishes this by connecting the (Koch\u2010carbonylation\u2010led) direct and dual cycle mechanisms, which operate during the early and steady\u2010state phases of MTH catalysis, respectively. To unravel these mechanistic intricacies, we have performed catalytic and operando (i.e., UV\/Vis coupled with an online mass spectrometer) and solid\u2010state NMR spectroscopic\u2010based investigations on the MTH process, involving co\u2010feeding methanol and acetone (cf. a key Koch\u2010carbonylated species), including selective isotope\u2010labeling studies. Our iterative research approach revealed that (Koch\u2212)carbonyl group selectively promotes the side\u2010chain mechanism within the arene cycle of the dual cycle mechanism, impacting the preferential formation of BTX fraction (i.e., benzene\u2010toluene\u2010xylene) primarily.<\/jats:p>","DOI":"10.1002\/anie.202318250","type":"journal-article","created":{"date-parts":[[2024,1,23]],"date-time":"2024-01-23T03:53:28Z","timestamp":1705982008000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Tracking the Impact of Koch\u2010Carbonylated Organics During the Zeolite ZSM\u20105 Catalyzed Methanol\u2010to\u2010Hydrocarbons Process"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-9910-7540","authenticated-orcid":false,"given":"Hexun","family":"Zhou","sequence":"first","affiliation":[{"name":"College of Chemistry and Molecular Sciences Wuhan University  Wuhan 430072 Hubei P. R. 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