Xiaoyun Dong, Fulin Zhang, Yuexin Wang, Fengwei Huang, Xianjun Lang
{"title":"用 TEMPO 在芘共价有机框架光催化剂上用氧选择性氧化硫化物","authors":"Xiaoyun Dong, Fulin Zhang, Yuexin Wang, Fengwei Huang, Xianjun Lang","doi":"10.1016/j.apcatb.2023.123660","DOIUrl":null,"url":null,"abstract":"<div><p><span>Covalent organic frameworks (COFs) can be precisely modulated through the covalent linkage of organic building blocks. Therefore, developing COFs to high-performance photocatalysts is highly applicable. Herein, with trifluoroacetic acid as the catalyst, Py-Azine-COF is constructed by aldimine condensation between 1,3,6,8-tetrakis(4-formylphenyl)pyrene and hydrazine hydrate. The highly crystalline Py-Azine-COF possesses a remarkable specific surface area of 1428 m</span><sup>2</sup> g<sup>−1</sup><span><span>. Intriguingly, selective aerobic conversion is achieved over Py-Azine-COF photocatalyst with (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO). Significantly, TEMPO accelerates the hole transfer and cooperates with superoxide formed from oxygen for selective oxidation of organic sulfides. With the assistance of 2 mol% TEMPO, the performance of Py-Azine-COF photocatalyst is increased markedly. Gratifyingly, TEMPO, a hole mediator, enables expeditious conversions of various sulfides into sulfoxides over Py-Azine-COF photocatalyst in methanol. Generally, COFs can be customized by modulating the covalent connection of organic building blocks to meet the requirements of selective aerobic </span>oxidations.</span></p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"345 ","pages":"Article 123660"},"PeriodicalIF":20.2000,"publicationDate":"2023-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective oxidation of sulfides with oxygen over a pyrene covalent organic framework photocatalyst with TEMPO\",\"authors\":\"Xiaoyun Dong, Fulin Zhang, Yuexin Wang, Fengwei Huang, Xianjun Lang\",\"doi\":\"10.1016/j.apcatb.2023.123660\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p><span>Covalent organic frameworks (COFs) can be precisely modulated through the covalent linkage of organic building blocks. Therefore, developing COFs to high-performance photocatalysts is highly applicable. Herein, with trifluoroacetic acid as the catalyst, Py-Azine-COF is constructed by aldimine condensation between 1,3,6,8-tetrakis(4-formylphenyl)pyrene and hydrazine hydrate. The highly crystalline Py-Azine-COF possesses a remarkable specific surface area of 1428 m</span><sup>2</sup> g<sup>−1</sup><span><span>. Intriguingly, selective aerobic conversion is achieved over Py-Azine-COF photocatalyst with (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO). Significantly, TEMPO accelerates the hole transfer and cooperates with superoxide formed from oxygen for selective oxidation of organic sulfides. With the assistance of 2 mol% TEMPO, the performance of Py-Azine-COF photocatalyst is increased markedly. Gratifyingly, TEMPO, a hole mediator, enables expeditious conversions of various sulfides into sulfoxides over Py-Azine-COF photocatalyst in methanol. Generally, COFs can be customized by modulating the covalent connection of organic building blocks to meet the requirements of selective aerobic </span>oxidations.</span></p></div>\",\"PeriodicalId\":244,\"journal\":{\"name\":\"Applied Catalysis B: Environmental\",\"volume\":\"345 \",\"pages\":\"Article 123660\"},\"PeriodicalIF\":20.2000,\"publicationDate\":\"2023-12-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis B: Environmental\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926337323013036\",\"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":"Applied Catalysis B: Environmental","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926337323013036","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Selective oxidation of sulfides with oxygen over a pyrene covalent organic framework photocatalyst with TEMPO
Covalent organic frameworks (COFs) can be precisely modulated through the covalent linkage of organic building blocks. Therefore, developing COFs to high-performance photocatalysts is highly applicable. Herein, with trifluoroacetic acid as the catalyst, Py-Azine-COF is constructed by aldimine condensation between 1,3,6,8-tetrakis(4-formylphenyl)pyrene and hydrazine hydrate. The highly crystalline Py-Azine-COF possesses a remarkable specific surface area of 1428 m2 g−1. Intriguingly, selective aerobic conversion is achieved over Py-Azine-COF photocatalyst with (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO). Significantly, TEMPO accelerates the hole transfer and cooperates with superoxide formed from oxygen for selective oxidation of organic sulfides. With the assistance of 2 mol% TEMPO, the performance of Py-Azine-COF photocatalyst is increased markedly. Gratifyingly, TEMPO, a hole mediator, enables expeditious conversions of various sulfides into sulfoxides over Py-Azine-COF photocatalyst in methanol. Generally, COFs can be customized by modulating the covalent connection of organic building blocks to meet the requirements of selective aerobic oxidations.
期刊介绍:
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.