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

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yue Zhu, Zhouying Mao, Weixiang Wu, Buxing Han, Qingqing Mei
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引用次数: 0

摘要

废聚对苯二甲酸乙二醇酯(PET)的部分加氢为生产有价值的化学品提供了很好的机会,但实现精确的催化控制仍然具有挑战性。在此,我们首次使用特殊设计的PtW/MCM-48催化剂,实现了废PET一锅选择性加氢制对甲苯(p-TA),收率达到创纪录的53.4%,对二甲苯(PX)收率达到36.4%。机制研究表明,特殊的催化性能是由Pt纳米粒子与WOx物种之间的协同相互作用引起的。低价WOx增强了Pt的分散性,而Pt稳定WOx为低聚合的多钨酸盐。PtW1.5/MCM-48的酸度适中,可控制p-TA的解吸,防止过加氢生成PX。催化剂在真实的PET废料中表现出强劲的性能。生命周期评价和技术经济评价进一步突出了其实际可行性。本研究为PET化学升级回收建立了一条可持续的途径,并为设计用于选择性氢化反应的先进催化剂提供了框架,解决了循环化学和塑料废物管理中的关键挑战。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Selective Asymmetric Hydrogenation of Waste Polyethylene Terephthalate via Controlled Sorption through Precisely Tuned Moderate Acid Sites

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.
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
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.
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