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通过负载钌催化剂将芳香族聚合物废料选择性升级循环转化为轻质碳-碳芳烃

Selective Upcycling of Aromatic Polymer Waste into Light CC Aromatics Over Ru-Supported Catalysts.

作者信息

Manal Arjun K, Zhao Jun, Bal Rajaram, Srivastava Rajendra

机构信息

Catalysis Research Laboratory, Department of Chemistry, Indian Institute of Technology Ropar, Rupnagar, Punjab, 140001, India.

Department of Biology, Institute of Advanced Materials, Hong Kong Baptist University, Kowloon Tong, Hong Kong SAR, China.

出版信息

ChemSusChem. 2025 Jul 27;18(15):e202500902. doi: 10.1002/cssc.202500902. Epub 2025 Jun 27.

DOI:10.1002/cssc.202500902
PMID:40454548
Abstract

The valorization of plastic waste and biomass has gained significant attention in the twenty first century. Despite structural similarities and the potential to yield similar products, an integrated approach to converting both feedstocks using the same catalyst has not been realized. This study demonstrates the catalytic upcycling of plastic waste and lignin biomass into selective CC aromatics through CO and/or CC bond cleavage using Ru-supported catalysts. The Ru/TiO exhibits remarkable performance, achieving 75%-90% yield from single, mixed plastic polymers and lignin. The exceptional activity of Ru/TiO stems from its unique structural and electronic properties. H spillover at the Ru-TiO interface transfers in the form of H/e, where the e reduces TiO to TiO, generating surface oxygen vacancies and inducing strong metal support interactions, while H migrates to the adjacent oxygen sites, forming new Brønsted acid sites. Oxygen vacancies at TiO sites promote the activation and cleavage of CO bonds, while Brønsted acid sites assist in the cleavage of CC bonds. Additionally, ultrasmall, highly dispersed Ru suppresses the hydrogenation of aromatics. These synergistic properties enable Ru/TiO to selectively produce aromatics, offering a promising strategy for catalytic upcycling of aromatic polymer waste into sustainable chemicals, aligning with the circular economy.

摘要

在21世纪,塑料废弃物和生物质的增值利用已备受关注。尽管二者在结构上有相似之处且有产出相似产品的潜力,但尚未实现采用相同催化剂对两种原料进行转化的综合方法。本研究展示了使用负载钌催化剂通过CO和/或CC键断裂将塑料废弃物和木质素生物质催化升级循环转化为选择性CC芳烃。Ru/TiO表现出卓越性能,从单一、混合塑料聚合物和木质素中实现了75% - 90%的产率。Ru/TiO的优异活性源于其独特的结构和电子性质。在Ru-TiO界面处的氢溢流以H/e的形式转移,其中e将TiO还原为TiO,产生表面氧空位并诱导强金属-载体相互作用,而H迁移至相邻的氧位点,形成新的布朗斯特酸位点。TiO位点处的氧空位促进CO键的活化和断裂,而布朗斯特酸位点协助CC键的断裂。此外,超小、高度分散的Ru抑制芳烃的氢化。这些协同性质使Ru/TiO能够选择性地生产芳烃,为将芳香聚合物废弃物催化升级循环转化为可持续化学品提供了一种有前景的策略,符合循环经济理念。

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