{"title":"基于磷酸的共价有机框架的微环境效应催化作用","authors":"Wenqi Qiu, Jialin Cui, Kejin Zhu, Meng Gao, Xuhan Zheng, Hui Liu, Zongxia Guo, Zhenxiu Zhang, Yingjie Zhao","doi":"10.1021/acscatal.4c04877","DOIUrl":null,"url":null,"abstract":"Drawing inspiration from enzymatic catalysis, a phosphoric acid-based covalent organic framework (<b>PA-COF</b>) was engineered for the efficient synthesis of optically pure lactide. <b>PA-COF</b> catalyst features precisely engineered microenvironments within well-defined porous channels decorated with phosphoric acid as the catalytically active sites. Much like enzymatic catalysis, where product selectivity is governed by the protein pocket, <b>PA-COF</b> provides precise microenvironments due to its highly ordered channels and adjustable structures. The phosphoric acids in the channels as catalytically active sites play key roles in directly converting lactic acid monomers into the cyclic dimer lactide. The process effectively avoided oligomerization, achieving an excellent yield of approximately 95%. This approach significantly differs from the traditional two-step strategy. It avoids the use of metal catalysts and high-temperature (∼200 °C) reaction conditions, thus avoiding metal residues and racemization. This microenvironment effect catalysis strategy provides a new pathway for the synthesis of lactide and may be extended to other useful condensation reactions.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":11.3000,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Microenvironment Effect Catalysis with Phosphoric Acid-Based Covalent Organic Frameworks\",\"authors\":\"Wenqi Qiu, Jialin Cui, Kejin Zhu, Meng Gao, Xuhan Zheng, Hui Liu, Zongxia Guo, Zhenxiu Zhang, Yingjie Zhao\",\"doi\":\"10.1021/acscatal.4c04877\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Drawing inspiration from enzymatic catalysis, a phosphoric acid-based covalent organic framework (<b>PA-COF</b>) was engineered for the efficient synthesis of optically pure lactide. <b>PA-COF</b> catalyst features precisely engineered microenvironments within well-defined porous channels decorated with phosphoric acid as the catalytically active sites. Much like enzymatic catalysis, where product selectivity is governed by the protein pocket, <b>PA-COF</b> provides precise microenvironments due to its highly ordered channels and adjustable structures. The phosphoric acids in the channels as catalytically active sites play key roles in directly converting lactic acid monomers into the cyclic dimer lactide. The process effectively avoided oligomerization, achieving an excellent yield of approximately 95%. This approach significantly differs from the traditional two-step strategy. It avoids the use of metal catalysts and high-temperature (∼200 °C) reaction conditions, thus avoiding metal residues and racemization. This microenvironment effect catalysis strategy provides a new pathway for the synthesis of lactide and may be extended to other useful condensation reactions.\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":null,\"pages\":null},\"PeriodicalIF\":11.3000,\"publicationDate\":\"2024-09-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acscatal.4c04877\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c04877","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Microenvironment Effect Catalysis with Phosphoric Acid-Based Covalent Organic Frameworks
Drawing inspiration from enzymatic catalysis, a phosphoric acid-based covalent organic framework (PA-COF) was engineered for the efficient synthesis of optically pure lactide. PA-COF catalyst features precisely engineered microenvironments within well-defined porous channels decorated with phosphoric acid as the catalytically active sites. Much like enzymatic catalysis, where product selectivity is governed by the protein pocket, PA-COF provides precise microenvironments due to its highly ordered channels and adjustable structures. The phosphoric acids in the channels as catalytically active sites play key roles in directly converting lactic acid monomers into the cyclic dimer lactide. The process effectively avoided oligomerization, achieving an excellent yield of approximately 95%. This approach significantly differs from the traditional two-step strategy. It avoids the use of metal catalysts and high-temperature (∼200 °C) reaction conditions, thus avoiding metal residues and racemization. This microenvironment effect catalysis strategy provides a new pathway for the synthesis of lactide and may be extended to other useful condensation reactions.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.