{"title":"用于高效光催化的亚胺连接苯并噻唑基共价有机框架的结构调控","authors":"Xin Zhao, Yuancheng Wang, Guangchao Han, Guoye Yu, Guanshi Ren, Xiang Li, Tongyang Zhang, Lishui Sun, Yingjie Zhao","doi":"10.1007/s11426-024-2507-5","DOIUrl":null,"url":null,"abstract":"<div><p>Slightly structural variation often leads to huge changes in the properties of the covalent organic frameworks (COFs). The atom-level precisely arranged structures of COFs make it possible to understand the structure-performance relationship. Here, four highly crystalline imine-linked benzothiadiazole-based COFs were constructed from precisely designed monomers. The effects of imine linkage orientation, the π bridge between the benzothiadiazole unit and imine linkage on the photocatalysis performance were systematically studied. It is noted that photocatalytic performance can be dramatically improved when the imine carbon atoms are attached to the pyrene-based unit. In addition, the extension of the π bridge in the benzothiadiazole units could obviously enhance the photocatalytic hydrogen evolution and weaken the hydrogen peroxide generation. The PC-NPB containing the diphenylbenzothiadiazole building block exhibited the highest hydrogen evolution rate of 15.7 mmol h<sup>−1</sup> g<sup>−1</sup>, 4.4 times higher than that of non-phenyl-substituted benzothiadiazole-containing PC-NB. Interestingly, PC-NB displayed the highest hydrogen peroxide generation rate of 1376 µmol h<sup>−1</sup> g<sup>−1</sup>, 2.8 times higher than that of PC-NPB.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":772,"journal":{"name":"Science China Chemistry","volume":"68 8","pages":"3707 - 3713"},"PeriodicalIF":9.7000,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Structural regulation of imine-linked benzothiadiazole-based covalent organic frameworks for efficient photocatalysis\",\"authors\":\"Xin Zhao, Yuancheng Wang, Guangchao Han, Guoye Yu, Guanshi Ren, Xiang Li, Tongyang Zhang, Lishui Sun, Yingjie Zhao\",\"doi\":\"10.1007/s11426-024-2507-5\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Slightly structural variation often leads to huge changes in the properties of the covalent organic frameworks (COFs). The atom-level precisely arranged structures of COFs make it possible to understand the structure-performance relationship. Here, four highly crystalline imine-linked benzothiadiazole-based COFs were constructed from precisely designed monomers. The effects of imine linkage orientation, the π bridge between the benzothiadiazole unit and imine linkage on the photocatalysis performance were systematically studied. It is noted that photocatalytic performance can be dramatically improved when the imine carbon atoms are attached to the pyrene-based unit. In addition, the extension of the π bridge in the benzothiadiazole units could obviously enhance the photocatalytic hydrogen evolution and weaken the hydrogen peroxide generation. The PC-NPB containing the diphenylbenzothiadiazole building block exhibited the highest hydrogen evolution rate of 15.7 mmol h<sup>−1</sup> g<sup>−1</sup>, 4.4 times higher than that of non-phenyl-substituted benzothiadiazole-containing PC-NB. Interestingly, PC-NB displayed the highest hydrogen peroxide generation rate of 1376 µmol h<sup>−1</sup> g<sup>−1</sup>, 2.8 times higher than that of PC-NPB.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":772,\"journal\":{\"name\":\"Science China Chemistry\",\"volume\":\"68 8\",\"pages\":\"3707 - 3713\"},\"PeriodicalIF\":9.7000,\"publicationDate\":\"2025-03-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science China Chemistry\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s11426-024-2507-5\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science China Chemistry","FirstCategoryId":"1","ListUrlMain":"https://link.springer.com/article/10.1007/s11426-024-2507-5","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Structural regulation of imine-linked benzothiadiazole-based covalent organic frameworks for efficient photocatalysis
Slightly structural variation often leads to huge changes in the properties of the covalent organic frameworks (COFs). The atom-level precisely arranged structures of COFs make it possible to understand the structure-performance relationship. Here, four highly crystalline imine-linked benzothiadiazole-based COFs were constructed from precisely designed monomers. The effects of imine linkage orientation, the π bridge between the benzothiadiazole unit and imine linkage on the photocatalysis performance were systematically studied. It is noted that photocatalytic performance can be dramatically improved when the imine carbon atoms are attached to the pyrene-based unit. In addition, the extension of the π bridge in the benzothiadiazole units could obviously enhance the photocatalytic hydrogen evolution and weaken the hydrogen peroxide generation. The PC-NPB containing the diphenylbenzothiadiazole building block exhibited the highest hydrogen evolution rate of 15.7 mmol h−1 g−1, 4.4 times higher than that of non-phenyl-substituted benzothiadiazole-containing PC-NB. Interestingly, PC-NB displayed the highest hydrogen peroxide generation rate of 1376 µmol h−1 g−1, 2.8 times higher than that of PC-NPB.
期刊介绍：
Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field.
Categories of articles include:
Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry.
Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies.
Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.
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