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This work systematically studied the compatibility and effectiveness of plasma and thermocatalytic tandem systems. By optimizing the plasma process in a self\u2010designed dielectric barrier discharge (DBD) reactor, we enhanced methane conversion (68.0%), methanol concentration (5.2\u00a0mol\u00a0L\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), and CO selectivity (56.9%), while preventing carbon deposition and CO\n                    <jats:sub>2<\/jats:sub>\n                    formation. In subsequent thermocatalysis, we developed the stearic acid\u2010modified ReRh\/ZSM\u20105\u2010S hydrophobic catalyst to avoid the separation of methanol and CO from the mixture and minimize the influence of by\u2010products (e.g., H\n                    <jats:sub>2<\/jats:sub>\n                    O). This innovative approach achieved 52.0% CH\n                    <jats:sub>3<\/jats:sub>\n                    COOH selectivity and 1.3\u00a0mol\u00a0L\n                    <jats:sup>\u22121<\/jats:sup>\n                    concentrations, three orders of magnitude than traditional methods, meeting the preliminary industrial criteria. This study demonstrates the potential of tandem catalysis, offering valuable insights for the efficient utilization of methane and other challenging catalytic reactions.\n                  <\/jats:p>","DOI":"10.1002\/anie.202502822","type":"journal-article","created":{"date-parts":[[2025,4,7]],"date-time":"2025-04-07T17:01:41Z","timestamp":1744045301000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["A Novel Tandem Reaction System for High\u2010Concentration Acetic Acid Production from Methane and Oxygen"],"prefix":"10.1002","volume":"64","author":[{"given":"Haonan","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical Engineering &amp; Institute of New Energy China University of Petroleum (East China)  Qingdao 266580 P.R. 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