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Herein, we report a catalyst microenvironment engineering strategy that introduces frustrated Lewis pairs (FLP) characteristics into established high\u2010performance catalysts for unlocking their full catalytic potential, rather than relying on the development of entirely new catalytic materials. Using a Co\u2010based catalyst as an example, we demonstrated that the designed FLP\u2010CoO\n                    <jats:sub>x<\/jats:sub>\n                    catalyst, featuring abundant surface FLP sites, markedly enhances O\n                    <jats:sub>2<\/jats:sub>\n                    activation, enabling the efficient generation of superoxide radicals (O\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2022\u2212<\/jats:sup>\n                    ) via a single\u2010electron reduction pathway. As a result, an outstanding dicarboxylic acid carbon yield of up to 86.0% was achieved under mild conditions, representing a fourfold improvement over the conventional catalyst. Moreover, the catalytic system exhibited excellent performance toward the oxidative valorization of various real\u2010world waste plastics. This work presents FLP\u2010mediated catalyst microenvironment engineering as a general strategy for substantially enhancing the performance of existing catalysts, providing new opportunities for the oxidative upcycling of waste plastics.\n                  <\/jats:p>","DOI":"10.1002\/anie.7232174","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T03:45:23Z","timestamp":1790826323000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Frustrated Lewis Pairs Enable Efficient Polyethylene Oxidative Upcycling"],"prefix":"10.1002","author":[{"given":"Tingxi","family":"Chen","sequence":"first","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling School of the Environment Nanjing University  Nanjing China"},{"name":"Institute For the Environment and Health Nanjing University Suzhou Campus  Suzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huai\u2010Cong","family":"Hu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Centre For Computational Chemistry and Research Institute of Industrial Catalysis School of Chemistry and Molecular Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fan","family":"Yuan","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling School of the Environment Nanjing University  Nanjing China"},{"name":"Institute For the Environment and Health Nanjing University Suzhou Campus  Suzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuqin","family":"Hu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling School of the Environment Nanjing University  Nanjing China"},{"name":"Institute For the Environment and Health Nanjing University Suzhou Campus  Suzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mengying","family":"Zheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling School of the Environment Nanjing University  Nanjing China"},{"name":"Institute For the Environment and Health Nanjing University Suzhou Campus  Suzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaolei","family":"Qu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling School of the Environment Nanjing University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhi\u2010Qiang","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Green Chemical Engineering and Industrial Catalysis Centre For Computational Chemistry and Research Institute of Industrial Catalysis School of Chemistry and Molecular Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9747-3044","authenticated-orcid":false,"given":"Yaxuan","family":"Jing","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling School of the Environment Nanjing University  Nanjing China"},{"name":"Institute For the Environment and Health Nanjing University Suzhou Campus  Suzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,9,30]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41570\u2010022\u201000411\u20108"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c04848"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/D5EE07522J"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.5c06816"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c13265"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44286\u2010024\u201000121\u20106"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c09153"},{"key":"e_1_2_8_9_1","first-page":"305","article-title":"Recent Advances in the Chemical Transformation of Polyolefins Into Small Molecules","volume":"57","author":"Yu Y. 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