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Polydiketoenamines (PDKs) are recyclable alternatives; however, monomers such as dimedone are petrochemical-derived and offer limited tunability. We computationally screened 144 \u03b2-keto-\u03b4-lactones (BKDLs), identifying solvation free energy as the primary determinant of depolymerization temperature across a 20\u201360\u2009\u00b0C range. We engineered hybrid type I polyketide synthases (PKSs) in\n                    <jats:italic>Escherichia<\/jats:italic>\n                    <jats:italic>coli<\/jats:italic>\n                    and\n                    <jats:italic>Streptomyces<\/jats:italic>\n                    hosts to biosynthesize BKDLs with diverse substituents and defined stereochemistry, reaching titers of 1.84\u2009g\u2009L\n                    <jats:sup>\u22121<\/jats:sup>\n                    in bioreactors. Polymerization of chemically synthesized BKDLs identical to PKS products confirmed tunable glass transition temperatures (53\u201398\u2009\u00b0C) and temperature-gated depolymerization. Different BKDLs yielded PDKs with thermal, mechanical, solvent-resistance and optical properties governed by substituent and chirality. Technoeconomic and life-cycle analyses indicate that corn-stover-derived BKDLs can outperform petrochemical dimedone on cost and greenhouse gas emissions. This study demonstrates that engineered PKSs can produce monomers for recyclable plastics with programmable depolymerization behavior.\n                  <\/jats:p>","DOI":"10.1038\/s41587-026-03229-7","type":"journal-article","created":{"date-parts":[[2026,7,27]],"date-time":"2026-07-27T09:02:04Z","timestamp":1785142924000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Engineered polyketide synthases enable a microbial chassis for recyclable plastics with tunable properties"],"prefix":"10.1038","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-4414-9494","authenticated-orcid":false,"given":"Zilong","family":"Wang","sequence":"first","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Seokjung","family":"Cheong","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1215-2613","authenticated-orcid":false,"given":"Hai","family":"Wang","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0311-3575","authenticated-orcid":false,"given":"Jeremy","family":"Demarteau","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9914-2388","authenticated-orcid":false,"given":"Alexander R.","family":"Epstein","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6309-0088","authenticated-orcid":false,"given":"Baishakhi","family":"Bose","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Weixi","family":"Hu","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3363-4777","authenticated-orcid":false,"given":"Matthias","family":"Schmidt","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-1098-655X","authenticated-orcid":false,"given":"Leah","family":"Keiser","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Mei","family":"Zhao","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Beibei","family":"Ge","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Alberto A.","family":"Nava","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Ramu","family":"Kakumanu","sequence":"additional","affiliation":[],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Edward E. 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B.A.H., J.D.K. and C.D.S. have financial interest in Cyklos Materials. Z.W. and S.C. have financial interest in FutureBio. The other authors declare no competing interests.","order":1,"name":"Ethics","label":"Competing interests","group":{"name":"EthicsHeading","label":"Ethics"}}]}}