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However, conventional bioproduction of homopolymeric P4HB involves complex and costly processes with C4 feedstocks, particularly 1,4\u2010butanediol (BDO), and enzyme\u2010coenzyme systems in genetically engineered bacteria. An alternative extracellular chemical route utilizing aerial oxidation of BDO offers cost and energy benefits but struggle with conversion efficiency. Inspired by efficient intracellular oxidation of primary alcohols, we propose a ruthenium\u2010phosphine synergistic catalytic system that mimics enzyme\u2010coenzyme functionality. This system effectively catalyzed the air\u2010mediated, solvent\u2010free oxidation of BDO to produce \u03b3\u2010butyrolactone (\u03b3\u2010BL) and oligomeric P4HB, with a space\u2010time yield (10.37\u2005g [\u03b3\u2010BL unit] g<jats:sup>\u22121<\/jats:sup> catalyst h<jats:sup>\u22121<\/jats:sup>) surpassing the values (&lt;5.5) of previous approaches. The oligomer\u2010containing products were reversibly converted to \u03b3\u2010BL and then to P4HB (28.9\u2005kDa) via ring\u2010opening polymerization, exceeding reported values (&lt;16\u2005kDa). This study provides the potential for large\u2010scale synthesis of high\u2010value PHAs from diverse non\u2010grain\u2010based diols, offering economic and environmental advantages.<\/jats:p>","DOI":"10.1002\/anie.202417660","type":"journal-article","created":{"date-parts":[[2024,12,23]],"date-time":"2024-12-23T10:59:03Z","timestamp":1734951543000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Air\u2010Mediated Biomimetic Synthesis of Polyhydroxyalkanoate with C4 Diol"],"prefix":"10.1002","volume":"64","author":[{"given":"Huilin","family":"Xie","sequence":"first","affiliation":[{"name":"Advanced Functional Materials Research Center Chemistry and Chemical Engineering Guangdong Laboratory  515031 Shantou China"},{"name":"College of Chemistry and Chemical Engineering Shantou University  515063 Shantou 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