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The key challenge is to control pathway selection across consecutive decarboxylation steps, favoring sequential aryl\u2013carboxyl C\u2013C bond cleavage over competing hydrogenolysis while preserving the aromatic core. Herein, we report an efficient direct catalytic conversion of waste PET to benzene, achieving an exceptionally high yield of 83.3% over a tailored Ru\/W0.4ZrOx catalyst. The performance arises from synergistic acid-site reconstruction and oxygen-vacancy engineering. Moderate WOx incorporation into ZrO2 converts Lewis acidity into Br\u00f8nsted acidity, while oxygen vacancies and WOx species promote adsorption and activation of carboxyl groups. In cooperation with Ru nanoparticles, these features preferentially stabilize the decarboxylation intermediate over its hydrogenolysis counterpart, directing both consecutive steps toward C\u2013C bond cleavage while suppressing undesired hydrogenolysis pathways. Controlled hydrogen supply and a deliberately designed dodecane\/water mixed solvent system further enhance selectivity. The catalyst performs effectively across diverse real-world PET wastes, with preliminary techno-economic and life-cycle analyses indicating favorable process-level metrics under the evaluated assumptions. More broadly, these mechanistic insights establish synergistic acidity and oxygen-vacancy regulation as a catalyst-design principle for decarboxylative skeletal editing of aromatic polycarboxylates.<\/jats:p>","DOI":"10.1021\/jacs.6c11537","type":"journal-article","created":{"date-parts":[[2026,10,10]],"date-time":"2026-10-10T15:01:48Z","timestamp":1791644508000},"page":"44380-44396","source":"Crossref","is-referenced-by-count":0,"title":["Selective Consecutive\nDecarboxylation Enables Skeletal\nContraction of Waste PET"],"prefix":"10.1021","volume":"148","author":[{"given":"Yue","family":"Zhu","sequence":"first","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310058"]},{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310058"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhouying","family":"Mao","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310058"]},{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310058"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0440-809X","authenticated-orcid":true,"given":"Buxing","family":"Han","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0210-1377","authenticated-orcid":true,"given":"Qingqing","family":"Mei","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310058"]},{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310058"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,10]]},"reference":[{"issue":"23","key":"2026102111065384300_cit1","doi-asserted-by":"publisher","first-page":"14625","DOI":"10.1021\/acscatal.1c03869","article-title":"On the Mechanism of Catalytic Decarboxylation of Carboxylic\nAcids on Carbon-Supported Palladium Hydride","volume":"11","author":"Deng","year":"2021","journal-title":"ACS Catal."},{"key":"2026102111065384300_cit2","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcat.2023.08.002","article-title":"Palladium Hydride\nPromotion by KHCO3 Enhances\nthe Decarboxylation Rate","volume":"427","author":"Deng","year":"2023","journal-title":"J. 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