{"title":"Predesign of Covalent‐Organic Frameworks for Efficient Photocatalytic Dehydrogenative Cross‐Coupling Reaction","authors":"Yu Chen, Sheng‐Nan Sun, Xiao‐Hong Chen, Ming‐Lin Chen, Jiao‐Min Lin, Qian Niu, Shun‐Li Li, Jiang Liu, Ya‐Qian Lan","doi":"10.1002/adma.202413638","DOIUrl":null,"url":null,"abstract":"The dehydrogenative cross‐coupling reaction is the premier route for synthesizing important 4‐quinazolinone drugs. However, it usually requires high reaction temperature and long reaction time, and the yield of the final product is low. Here two stable and photosensitive covalent‐organic frameworks (COFs), TAPP‐An and TAPP‐Cu‐An are purposefully designed and constructed to serve as unprecedented heterogeneous tandem catalysts to complete dehydrogenative cross‐coupling reactions in a short time and under mild reaction conditions (room temperature and light), leading to the high‐efficient photosynthesis of 4‐quinazolinones. Particularly, TAPP‐Cu‐An is the best heterogeneous catalyst currently available for the synthesis of 4‐quinazolinones, even surpassing all the catalysts reported so far. It also enables one‐step photosynthesis of 4‐quinazolinones with higher conversion (>99%) and selectivity (>99%) in a shorter time, and the product can be easily prepared on a gram scale. Extensive experiments combined with theoretical calculations show that the excellent photogenerated charge separation and transport capability, as well as the synergistic An‐Cu catalysis in TAPP‐Cu‐An are the main driving forces for this efficient reaction.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"13 1","pages":""},"PeriodicalIF":27.4000,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adma.202413638","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The dehydrogenative cross‐coupling reaction is the premier route for synthesizing important 4‐quinazolinone drugs. However, it usually requires high reaction temperature and long reaction time, and the yield of the final product is low. Here two stable and photosensitive covalent‐organic frameworks (COFs), TAPP‐An and TAPP‐Cu‐An are purposefully designed and constructed to serve as unprecedented heterogeneous tandem catalysts to complete dehydrogenative cross‐coupling reactions in a short time and under mild reaction conditions (room temperature and light), leading to the high‐efficient photosynthesis of 4‐quinazolinones. Particularly, TAPP‐Cu‐An is the best heterogeneous catalyst currently available for the synthesis of 4‐quinazolinones, even surpassing all the catalysts reported so far. It also enables one‐step photosynthesis of 4‐quinazolinones with higher conversion (>99%) and selectivity (>99%) in a shorter time, and the product can be easily prepared on a gram scale. Extensive experiments combined with theoretical calculations show that the excellent photogenerated charge separation and transport capability, as well as the synergistic An‐Cu catalysis in TAPP‐Cu‐An are the main driving forces for this efficient reaction.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.