Xu Chi, Zixing Zhang, Mengqi Li, Yang Jiao, Xiaomeng Li, Fancheng Meng, Bai Xue, Dongqing Wu, Fan Zhang
{"title":"用于 H2O2 合成的多环芳烃与 π-扩展二维共价有机框架光催化剂的乙烯连接","authors":"Xu Chi, Zixing Zhang, Mengqi Li, Yang Jiao, Xiaomeng Li, Fancheng Meng, Bai Xue, Dongqing Wu, Fan Zhang","doi":"10.1002/anie.202418895","DOIUrl":null,"url":null,"abstract":"Polycyclic aromatic hydrocarbons (PAHs) hold the predominant role either as individual molecules or building blocks in the field of organic semiconductors or nanocarbons. Connecting PAHs via sp2-carbon bridges to form high-crystalline p-extended structures is highly desired not only for enlarging the regimes of two-dimensional materials but also for achieving exceptional properties/functions. In this work, we developed 5,10-dimethyl-4,9-diazapyrene as a key monomer, whose two methyl groups at the positions adjacent to nitrogen atoms, can helpfully increase the solubility, and serve as the active connection sites. In the presence of organic acids, this monomer enables smoothly conducting Knoevenagel condensation to form two vinylene-linked PAH-cored COFs, which show high-crystalline honeycomb structures with large surface areas up to 1238 m2 g−1. Owing to the direct connection mode of PAH building blocks with vinylene, the as-prepared COFs possess spatially extended p-conjugation and substantial semiconducting properties. Consequently, their visible-light photocatalysis with exceptional activity and durability was manifested to generate H2O2 up to 3820 µmol g-1 h-1 in pure water, and even 17080 µmol g-1 h-1 using benzyl alcohol as a hole sacrificial agent.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":null,"pages":null},"PeriodicalIF":16.1000,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Vinylene-Linking of Polycyclic Aromatic Hydrocarbons to π-Extended Two-Dimensional Covalent Organic Framework Photocatalyst for H2O2 Synthesis\",\"authors\":\"Xu Chi, Zixing Zhang, Mengqi Li, Yang Jiao, Xiaomeng Li, Fancheng Meng, Bai Xue, Dongqing Wu, Fan Zhang\",\"doi\":\"10.1002/anie.202418895\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Polycyclic aromatic hydrocarbons (PAHs) hold the predominant role either as individual molecules or building blocks in the field of organic semiconductors or nanocarbons. Connecting PAHs via sp2-carbon bridges to form high-crystalline p-extended structures is highly desired not only for enlarging the regimes of two-dimensional materials but also for achieving exceptional properties/functions. In this work, we developed 5,10-dimethyl-4,9-diazapyrene as a key monomer, whose two methyl groups at the positions adjacent to nitrogen atoms, can helpfully increase the solubility, and serve as the active connection sites. In the presence of organic acids, this monomer enables smoothly conducting Knoevenagel condensation to form two vinylene-linked PAH-cored COFs, which show high-crystalline honeycomb structures with large surface areas up to 1238 m2 g−1. Owing to the direct connection mode of PAH building blocks with vinylene, the as-prepared COFs possess spatially extended p-conjugation and substantial semiconducting properties. Consequently, their visible-light photocatalysis with exceptional activity and durability was manifested to generate H2O2 up to 3820 µmol g-1 h-1 in pure water, and even 17080 µmol g-1 h-1 using benzyl alcohol as a hole sacrificial agent.\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":16.1000,\"publicationDate\":\"2024-10-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie International Edition\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1002/anie.202418895\",\"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":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202418895","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Vinylene-Linking of Polycyclic Aromatic Hydrocarbons to π-Extended Two-Dimensional Covalent Organic Framework Photocatalyst for H2O2 Synthesis
Polycyclic aromatic hydrocarbons (PAHs) hold the predominant role either as individual molecules or building blocks in the field of organic semiconductors or nanocarbons. Connecting PAHs via sp2-carbon bridges to form high-crystalline p-extended structures is highly desired not only for enlarging the regimes of two-dimensional materials but also for achieving exceptional properties/functions. In this work, we developed 5,10-dimethyl-4,9-diazapyrene as a key monomer, whose two methyl groups at the positions adjacent to nitrogen atoms, can helpfully increase the solubility, and serve as the active connection sites. In the presence of organic acids, this monomer enables smoothly conducting Knoevenagel condensation to form two vinylene-linked PAH-cored COFs, which show high-crystalline honeycomb structures with large surface areas up to 1238 m2 g−1. Owing to the direct connection mode of PAH building blocks with vinylene, the as-prepared COFs possess spatially extended p-conjugation and substantial semiconducting properties. Consequently, their visible-light photocatalysis with exceptional activity and durability was manifested to generate H2O2 up to 3820 µmol g-1 h-1 in pure water, and even 17080 µmol g-1 h-1 using benzyl alcohol as a hole sacrificial agent.
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.