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Notably, the direct one\u2010pot conversion of lignin into valuable compounds is crucial for advancing biomass utilization, aiming to streamline production by combining depolymerization and functionalization steps to maximize process\u2010, atom\u2010, and cost\u2010efficiency. Here we report the photocatalytic approach for synchronized depolymerization and C\u2013C coupling processes for the direct conversion of lignin and its derivatives into aromatic diols using CdZnS (Cd\n                    <jats:sub>0.3<\/jats:sub>\n                    Zn\n                    <jats:sub>0.7<\/jats:sub>\n                    S) catalyst. By coupling hole\u2010driven radical generation with electron\u2010driven regeneration of overoxidized benzylic intermediates, this strategy overcomes the intrinsic preference for homocoupling and enables selective cross\u2010coupling between benzylic and aliphatic alcohol derivatives. This CdZnS\u2010based photocatalytic process enables simultaneous hydrogen transfer, hydrogenolysis and cross\u2010coupling of various lignin model compounds with alcohols to obtain unsymmetrical aromatic diols. In the case of real lignin, this depolymerization\u2010cross\u2010coupling protocol gives corresponding aromatic diols up to 10\u00a0wt% monomer yield. The resulting diol products are directly applicable to the synthesis of thermoplastic polyurethanes (TPUs) as well as fused polycyclic frameworks, functional materials, and bioactive molecules.\n                  <\/jats:p>","DOI":"10.1002\/anie.2045478","type":"journal-article","created":{"date-parts":[[2026,6,9]],"date-time":"2026-06-09T11:56:35Z","timestamp":1781006195000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Photocatalytic Lignin Depolymerization and Cross\u2010Coupling With Alcohols to Produce Unsymmetric Aromatic Diols"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2360-1808","authenticated-orcid":false,"given":"Hongji","family":"Li","sequence":"first","affiliation":[{"name":"College of Chemistry Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jialing","family":"Ma","sequence":"additional","affiliation":[{"name":"College of Chemistry Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoling","family":"Wan","sequence":"additional","affiliation":[{"name":"College of Chemistry Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yumei","family":"Liu","sequence":"additional","affiliation":[{"name":"Leibniz\u2010Institut F\u00fcr Katalyse e.V.  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Rostock Germany"},{"name":"Nanotechnology Centre Centre for Energy and Environmental Technologies VS \u030cB\u2010Technical University of Ostrava  Ostrava\u2010Poruba Czech 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