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This work reveals the potential of a one\u2010pot catalytic lignin \u03b2\u2010O\u20104 depolymerization cascade strategy that yields a uniform set of methoxylated aromatics without alkyl side\u2010chains. This cascade consists of the selective acceptorless dehydrogenation of the \u03b3\u2010hydroxy group, a subsequent retro\u2010aldol reaction that cleaves the C\n                    <jats:sub>\u03b1<\/jats:sub>\n                    \u2212C\n                    <jats:sub>\u03b2<\/jats:sub>\n                    bond, followed by in situ acceptorless decarbonylation of the formed aldehydes. This three\u2010step cascade reaction, catalyzed by an iridium(I)\u2010BINAP complex, resulted in 75\u2009% selectivity for 1,2\u2010dimethoxybenzene from G\u2010type lignin dimers, alongside syngas (CO\u2009:\u2009H\n                    <jats:sub>2<\/jats:sub>\n                    \u22481.4\u2009:\u20091). Applying this method to a synthetic G\u2010type polymer, 11\u2005wt\u2009% 1,2\u2010dimethoxybenzene was obtained. This versatile compound can be easily transformed into 3,4\u2010dimethoxyphenol, a valuable precursor for pharmaceutical synthesis, through an enzymatic catalytic approach. Moreover, the hydrodeoxygenation potential of 1,2\u2010dimethoxybenzene offers a pathway to produce valuable cyclohexane or benzene derivatives, presenting enticing opportunities for sustainable chemical transformations without the necessity for phenolic mixture upgrading via dealkylation.\n                  <\/jats:p>","DOI":"10.1002\/anie.202410382","type":"journal-article","created":{"date-parts":[[2024,7,31]],"date-time":"2024-07-31T10:49:30Z","timestamp":1722422970000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["One\u2010Pot Catalytic Cascade for the Depolymerization of the Lignin \u03b2\u2010O\u20104 Motif to Non\u2010phenolic Dealkylated Aromatics"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-7776-5800","authenticated-orcid":false,"given":"Zhenlei","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering and Environment China University of Petroleum (Beijing)  102249 Beijing China"},{"name":"Department of Chemical Engineering (ENTEG) University of Groningen  Nijenborgh 4 9747 AG Groningen The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ge","family":"Guo","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering (ENTEG) University of Groningen  Nijenborgh 4 9747 AG Groningen The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huaizhou","family":"Yang","sequence":"additional","affiliation":[{"name":"Department of Chemical Engineering (ENTEG) University of Groningen  Nijenborgh 4 9747 AG Groningen The Netherlands"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lina","family":"Csechala","sequence":"additional","affiliation":[{"name":"Department of Biotechnology &amp; 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