Minhao Tang, Ji Shen, Fengtao Zhang, Yanfei Zhao, Tao Gan, Wei Zeng, Rongxiang Li, Dingsheng Wang, Buxing Han, Zhimin Liu
{"title":"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。","authors":"Minhao Tang, Ji Shen, Fengtao Zhang, Yanfei Zhao, Tao Gan, Wei Zeng, Rongxiang Li, Dingsheng Wang, Buxing Han, Zhimin Liu","doi":"10.1002/anie.202416436","DOIUrl":null,"url":null,"abstract":"<p><p>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 H<sub>2</sub> in acetic acid under mild conditions (e.g., 180 °C), which is achieved over anatase TiO<sub>2</sub> 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.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":19.3000,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Upcycling of Polyamide Wastes to Tertiary Amines Using Mo Single Atoms and Rh Nanoparticles.\",\"authors\":\"Minhao Tang, Ji Shen, Fengtao Zhang, Yanfei Zhao, Tao Gan, Wei Zeng, Rongxiang Li, Dingsheng Wang, Buxing Han, Zhimin Liu\",\"doi\":\"10.1002/anie.202416436\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>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 H<sub>2</sub> in acetic acid under mild conditions (e.g., 180 °C), which is achieved over anatase TiO<sub>2</sub> 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.</p>\",\"PeriodicalId\":16,\"journal\":{\"name\":\"ACS Energy Letters \",\"volume\":null,\"pages\":null},\"PeriodicalIF\":19.3000,\"publicationDate\":\"2024-10-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Energy Letters \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1002/anie.202416436\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Energy Letters ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202416436","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Upcycling of Polyamide Wastes to Tertiary Amines Using Mo Single Atoms and Rh Nanoparticles.
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.
ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment
CiteScore
31.20
自引率
5.00%
发文量
469
审稿时长
1 months
期刊介绍:
ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format.
ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology.
The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.