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Amino acid (AA) polymers, an important class of polyamides, provide an attractive molecular platform for constructing recyclable polymer systems. However, classical synthetic methods for AA polymers typically involve CO2 emissions and suffer from slow polymerization rate, poor controllability, and difficulty in achieving high molecular weight. Herein, we develop a CO2-mediated synthetic strategy for AA polymers using carbamates as reactive intermediates. This strategy not only enables the ultrafast synthesis of N-carboxyanhydride (NCA) monomers from CO2 and amino acids within 1 min under mild conditions, but also realizes a robust carbamate initiation strategy for the ultrafast and controlled NCA polymerization to afford AA polymers in a short time with predictable molecular weights. The carbamate initiator exhibits high reactivity and superior stability, enabling the facile synthesis of 21-block copolymers and high-molecular-weight AA polymers with diversified structures. Mechanistic studies revealed a distinct \u201cconcerted nucleophilic addition and decarboxylation\u201d polymerization pathway. Notably, the CO2 released during polymerization is simultaneously recycled for monomer and carbamate regeneration, forming a \u201cfixation\u2013release\u2013reuse\u201d closed-loop carbon cycle. The resulting AA polymer exhibited excellent processability with a high mechanical strength of 25.7 MPa, and could be efficiently depolymerized into amino acids with a recovery rate of 91.2%, demonstrating great potential as sustainable engineering plastics and biomaterials for circular polymer economies.<\/jats:p>","DOI":"10.1021\/jacs.6c17448","type":"journal-article","created":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T11:02:36Z","timestamp":1791543756000},"page":"45136-45146","source":"Crossref","is-referenced-by-count":0,"title":["Closed-Loop CO2-Mediated Ultrafast\nand Controlled Synthesis of Amino Acid Polymers toward a Circular\nCarbon and Polymer Economy"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9494-2685","authenticated-orcid":true,"given":"Kang","family":"Chen","sequence":"first","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]},{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]},{"name":"Suzhou Institute of Biomedical Engineering and Technology, Chinese Academy of Sciences , ,","place":["Suzhou, China, 215163"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yueming","family":"Wu","sequence":"additional","affiliation":[{"name":"Shanghai JiaoTong University , , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinqi","family":"Huang","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyi","family":"Xie","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawei","family":"Zeng","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lanrong","family":"Li","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7699-086X","authenticated-orcid":true,"given":"Runhui","family":"Liu","sequence":"additional","affiliation":[{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]},{"name":"East China University of Science and Technology , , ,","place":["Shanghai, China, 200237"]},{"name":"Suzhou Institute of Biomedical Engineering and Technology, Chinese Academy of Sciences , ,","place":["Suzhou, China, 215163"]},{"name":"Shanghai JiaoTong University , , ,","place":["Shanghai, China, 200240"]},{"name":"Shanghai Academy of Natural Sciences (SANS) , ,","place":["Shanghai, China, 200031"]},{"name":"Shanghai Shyndec Pharmaceutical Co., Ltd. , 378 Jian-Lu Road , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,9]]},"reference":[{"issue":"7997","key":"2026102111083903400_cit1","doi-asserted-by":"publisher","first-page":"45","DOI":"10.1038\/s41586-023-06939-z","article-title":"Designing a circular\ncarbon and plastics economy for a sustainable future","volume":"626","author":"Vidal","year":"2024","journal-title":"Nature"},{"issue":"5","key":"2026102111083903400_cit2","doi-asserted-by":"publisher","first-page":"2617","DOI":"10.1021\/acs.chemrev.3c00739","article-title":"Depolymerization\nwithin a circular plastics system","volume":"124","author":"Clark","year":"2024","journal-title":"Chem. 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