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The activity of different Cu\u2010sites for methane transformation is still under discussion. Herein, ZSM\u20105 zeolite has been loaded with Cu<jats:sup>2+<\/jats:sup> cations (1.4\u2005wt\u2009% Cu) as characterized by UV\u2010vis DRS, EPR, EXAFS, and <jats:sup>1<\/jats:sup>H MAS NMR. It is inferred that Cu<jats:sup>2+<\/jats:sup> cations, attached to the cation\u2010exchange Al\u2212O<jats:sup>\u2212<\/jats:sup>\u2212Si sites of the zeolite framework, can exist in the form of either isolated or paired Cu<jats:sup>2+<\/jats:sup> sites. The transformation of methane to methanol on Cu<jats:sup>2+<\/jats:sup>\/H\u2010ZSM\u20105 has been verified by the observation of the methoxy species formation with <jats:sup>13<\/jats:sup>C MAS NMR and FTIR spectroscopy. The related mechanisms have been analyzed by DFT calculations. The calculations show that the paired Cu<jats:sup>2+<\/jats:sup> sites enable heterolytic C\u2212H bond dissociation via the \u201calkyl\u201d pathway resulting in methylcopper species, which however are not detected experimentally due to further rapid transformation to surface methoxy species through methyl radical formation and recombination with Si\u2212O<jats:sup>\u2212<\/jats:sup>Al site. Based on the obtained data, it has been concluded that methane transformation to methanol on paired Cu<jats:sup>2+<\/jats:sup> sites, having no extra\u2010framework oxygen ligand, is possible in Cu\u2010modified zeolites. The pathways of Cu<jats:sup>2+<\/jats:sup> cations regeneration with O<jats:sub>2<\/jats:sub> and H<jats:sub>2<\/jats:sub>O have been experimentally explored.<\/jats:p>","DOI":"10.1002\/chem.202403167","type":"journal-article","created":{"date-parts":[[2025,1,9]],"date-time":"2025-01-09T01:48:28Z","timestamp":1736387308000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Methane to Methanol Transformation on Cu<sup>2+<\/sup>\/H\u2010ZSM\u20105 Zeolite. 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