PMID- 36524740 OWN - NLM STAT- MEDLINE DCOM- 20221229 LR - 20230104 IS - 1520-5126 (Electronic) IS - 0002-7863 (Linking) VI - 144 IP - 51 DP - 2022 Dec 28 TI - Catalytic Chemical Recycling of Post-Consumer Polyethylene. PG - 23280-23285 LID - 10.1021/jacs.2c11949 [doi] AB - Among commercial plastics, polyolefins are the most widely produced worldwide but have limited recyclability. Here, we report a chemical recycling route for the conversion of post-consumer high-density polyethylene (HDPE) into telechelic macromonomers suitable for circular reprocessing. Unsaturation was introduced into HDPE by catalytic dehydrogenation using an Ir-POCOP catalyst without an alkene acceptor. Cross-metathesis with 2-hydroxyethyl acrylate followed by hydrogenation transformed the partially unsaturated HDPE into telechelic macromonomers. The direct repolymerization of the macromonomers gave a brittle material due to the low overall weight-average molecular weight. Aminolysis of telechelic macromonomers with a small amount of diethanolamine increased the overall functionality. The resulting macromonomers were repolymerized through transesterification to generate a polymer with comparable mechanical properties to the starting post-consumer HDPE waste. Depolymerization of the repolymerized material catalyzed by an organic base regenerated the telechelic macromonomers, thereby allowing waste polyethylene materials to enter a chemical recycling pathway. FAU - Arroyave, Alejandra AU - Arroyave A AD - Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439-4801, United States. FAU - Cui, Shilin AU - Cui S AUID- ORCID: 0000-0002-6777-7688 AD - Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, United States. FAU - Lopez, Jaqueline C AU - Lopez JC AD - Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, United States. FAU - Kocen, Andrew L AU - Kocen AL AUID- ORCID: 0000-0001-8879-2011 AD - Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, United States. FAU - LaPointe, Anne M AU - LaPointe AM AUID- ORCID: 0000-0002-7830-0922 AD - Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, United States. FAU - Delferro, Massimiliano AU - Delferro M AUID- ORCID: 0000-0002-4443-165X AD - Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439-4801, United States. AD - Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637-1433, United States. FAU - Coates, Geoffrey W AU - Coates GW AUID- ORCID: 0000-0002-3400-2552 AD - Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, United States. LA - eng PT - Journal Article PT - Research Support, U.S. Gov't, Non-P.H.S. DEP - 20221216 PL - United States TA - J Am Chem Soc JT - Journal of the American Chemical Society JID - 7503056 RN - 9002-88-4 (Polyethylene) RN - 0 (Plastics) RN - 0 (Polymers) RN - 0 (Waste Products) SB - IM MH - *Polyethylene MH - *Plastics MH - Polymers MH - Waste Products MH - Catalysis EDAT- 2022/12/17 06:00 MHDA- 2022/12/30 06:00 CRDT- 2022/12/16 08:03 PHST- 2022/12/17 06:00 [pubmed] PHST- 2022/12/30 06:00 [medline] PHST- 2022/12/16 08:03 [entrez] AID - 10.1021/jacs.2c11949 [doi] PST - ppublish SO - J Am Chem Soc. 2022 Dec 28;144(51):23280-23285. doi: 10.1021/jacs.2c11949. Epub 2022 Dec 16.