Upcycling of Polyamide Wastes to Tertiary Amines Using Mo Single Atoms and Rh Nanoparticles

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2024-10-17 DOI:10.1002/anie.202416436
Dr. Minhao Tang, Ji Shen, Dr. Fengtao Zhang, Prof. Yanfei Zhao, Dr. Tao Gan, Dr. Wei Zeng, Rongxiang Li, Prof. Dingsheng Wang, Prof. Buxing Han, Prof. Zhimin Liu
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Abstract

The pursuit of sustainable practices through the chemical recycling of polyamide wastes holds significant potential, particularly in enabling the recovery of a range of nitrogen-containing compounds. Herein, we report a novel strategy to upcycle polyamide wastes to tertiary amines with the assistance of H2 in acetic acid under mild conditions (e.g., 180 °C), which is achieved over anatase TiO2 supported Mo single atoms and Rh nanoparticles. In this protocol, the polyamide is first converted into diacetamide intermediates via acidolysis, which are subsequently hydrogenated into corresponding carboxylic acid monomers and tertiary amines in 100 % selectivity. It is verified that Mo single atoms and Rh nanoparticles work together to activate both amide bonds of the diacetamide intermediate, and synergistically catalyze its hydrodeoxygenation to form tertiary amine, but this catalyst is ineffective for hydrogenation of carboxylic acid. This work presents an effective way to reconstruct various polyamide wastes into tertiary amines and carboxylic acids, which may have promising application potential.

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利用钼单原子和铑纳米颗粒将聚酰胺废料升级再造为叔胺。
通过对聚酰胺废料进行化学回收利用来实现可持续发展具有巨大潜力,特别是在回收一系列含氮化合物方面。在此,我们报告了一种新型策略,即在温和条件下(如 180 ºC),借助乙酸中的 H2,在支持 Mo 单原子和 Rh 纳米颗粒的锐钛型二氧化钛上,将聚酰胺废料升级回收为叔胺。在该方案中,聚酰胺首先通过酸解转化为二乙酰胺中间体,然后以 100% 的选择性氢化为相应的羧酸单体和叔胺。研究证实,Mo 单原子和 Rh 纳米粒子共同激活二乙酰胺中间体的两个酰胺键,并协同催化其氢脱氧生成叔胺,但这种催化剂对羧酸的氢化无效。这项研究提出了一种将各种聚酰胺废料重构为叔胺和羧酸的有效方法,具有广阔的应用前景。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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