Yue Zhu, Zhouying Mao, Weixiang Wu, Buxing Han, Qingqing Mei
{"title":"通过精确调节的中等酸位控制吸附,选择性不对称加氢废聚对苯二甲酸乙二醇酯","authors":"Yue Zhu, Zhouying Mao, Weixiang Wu, Buxing Han, Qingqing Mei","doi":"10.1021/jacs.5c01209","DOIUrl":null,"url":null,"abstract":"The partial hydrogenation of waste polyethylene terephthalate (PET) offers a great opportunity to produce valuable chemicals, yet achieving precise catalytic control remains challenging. Herein, for the first time, we realized one-pot selective hydrogenation of waste PET to <i>p</i>-toluic acid (<i>p</i>-TA) with a record-high yield of 53.4%, alongside a 36.4% yield of <i>p</i>-xylene (PX), using a specially designed PtW/MCM-48 catalyst. Mechanistic investigations revealed that the exceptional catalytic performance arises from synergistic interaction between Pt nanoparticles and WO<sub><i>x</i></sub> species. Low-valent WO<sub><i>x</i></sub> enhances Pt dispersion, while Pt stabilizes WO<sub><i>x</i></sub> as low-polymerized polytungstates. The moderate acidity of PtW<sub>1.5</sub>/MCM-48 ensures controlled desorption of <i>p</i>-TA, preventing overhydrogenation to PX. The catalyst demonstrated robust performance with real-world PET waste. Life cycle assessment and technical and economic evaluation further highlight its practical feasibility. This study establishes a sustainable pathway for PET chemical upcycling and provides a framework for designing advanced catalysts for selective hydrogenation reactions, addressing critical challenges in circular chemistry and plastic waste management.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"52 1","pages":""},"PeriodicalIF":15.6000,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective Asymmetric Hydrogenation of Waste Polyethylene Terephthalate via Controlled Sorption through Precisely Tuned Moderate Acid Sites\",\"authors\":\"Yue Zhu, Zhouying Mao, Weixiang Wu, Buxing Han, Qingqing Mei\",\"doi\":\"10.1021/jacs.5c01209\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The partial hydrogenation of waste polyethylene terephthalate (PET) offers a great opportunity to produce valuable chemicals, yet achieving precise catalytic control remains challenging. Herein, for the first time, we realized one-pot selective hydrogenation of waste PET to <i>p</i>-toluic acid (<i>p</i>-TA) with a record-high yield of 53.4%, alongside a 36.4% yield of <i>p</i>-xylene (PX), using a specially designed PtW/MCM-48 catalyst. Mechanistic investigations revealed that the exceptional catalytic performance arises from synergistic interaction between Pt nanoparticles and WO<sub><i>x</i></sub> species. Low-valent WO<sub><i>x</i></sub> enhances Pt dispersion, while Pt stabilizes WO<sub><i>x</i></sub> as low-polymerized polytungstates. The moderate acidity of PtW<sub>1.5</sub>/MCM-48 ensures controlled desorption of <i>p</i>-TA, preventing overhydrogenation to PX. The catalyst demonstrated robust performance with real-world PET waste. Life cycle assessment and technical and economic evaluation further highlight its practical feasibility. This study establishes a sustainable pathway for PET chemical upcycling and provides a framework for designing advanced catalysts for selective hydrogenation reactions, addressing critical challenges in circular chemistry and plastic waste management.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"52 1\",\"pages\":\"\"},\"PeriodicalIF\":15.6000,\"publicationDate\":\"2025-03-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.5c01209\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.5c01209","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Selective Asymmetric Hydrogenation of Waste Polyethylene Terephthalate via Controlled Sorption through Precisely Tuned Moderate Acid Sites
The partial hydrogenation of waste polyethylene terephthalate (PET) offers a great opportunity to produce valuable chemicals, yet achieving precise catalytic control remains challenging. Herein, for the first time, we realized one-pot selective hydrogenation of waste PET to p-toluic acid (p-TA) with a record-high yield of 53.4%, alongside a 36.4% yield of p-xylene (PX), using a specially designed PtW/MCM-48 catalyst. Mechanistic investigations revealed that the exceptional catalytic performance arises from synergistic interaction between Pt nanoparticles and WOx species. Low-valent WOx enhances Pt dispersion, while Pt stabilizes WOx as low-polymerized polytungstates. The moderate acidity of PtW1.5/MCM-48 ensures controlled desorption of p-TA, preventing overhydrogenation to PX. The catalyst demonstrated robust performance with real-world PET waste. Life cycle assessment and technical and economic evaluation further highlight its practical feasibility. This study establishes a sustainable pathway for PET chemical upcycling and provides a framework for designing advanced catalysts for selective hydrogenation reactions, addressing critical challenges in circular chemistry and plastic waste management.
期刊介绍:
The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.