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Current systems typically rely on Ru or Pt catalysts to mediate key elementary steps, including H\n                    <jats:sub>2<\/jats:sub>\n                    dissociation and C\u2500C bond cleavage. However, achieving comparable performance with earth\u2010abundant metals under near\u2010ambient hydrogen pressure remains a significant challenge. Here, we present an elementary reaction kinetic matching strategy to enable efficient hydrogenolysis over a non\u2010noble metal catalyst. By tuning the electronic structure of Ni, the kinetics of H\n                    <jats:sub>2<\/jats:sub>\n                    activation, C\u2500C bond cleavage, and hydrogenation are balanced, facilitating the rapid removal of CH\n                    <jats:sub>x<\/jats:sub>\n                    <jats:sup>*<\/jats:sup>\n                    intermediates and sustaining the dynamic exposure of catalytic active sites. As a result, the Ni\u2010based catalyst exhibited superior hydrogenolysis activity and selectivity toward waste polyolefins under low pressure, even at atmospheric pressure, surpassing the benchmark Ru and Pt catalysts. This study overturns the traditional perception of low efficiency in non\u2010noble metal\u2010catalyzed hydrogenolysis and provides new design principles for efficient catalysis under mild conditions.\n                  <\/jats:p>","DOI":"10.1002\/anie.9907362","type":"journal-article","created":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T10:32:06Z","timestamp":1788777126000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ambient\u2010Pressure Polyolefin Upcycling With Earth\u2010Abundant Catalyst"],"prefix":"10.1002","author":[{"given":"Qianyue","family":"Feng","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, Institute of Functional Nano &amp; Soft Materials (FUNSOM), Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University  Suzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingyu","family":"Chu","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Engineering, New Cornerstone Science Laboratory, College of Chemistry and Molecular Engineering Peking University Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhongyu","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, Institute of Functional Nano &amp; Soft Materials (FUNSOM), Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University  Suzhou P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9254-7430","authenticated-orcid":false,"given":"Jinxing","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Bioinspired Interfacial Materials Science, Institute of Functional Nano &amp; Soft Materials (FUNSOM), Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University  Suzhou P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3341-2998","authenticated-orcid":false,"given":"Ding","family":"Ma","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Engineering, New Cornerstone Science Laboratory, College of Chemistry and Molecular Engineering Peking University Beijing P. R. 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