Xiaoxiao Yu, Ke Gong, Shuyao Tian, Guangpeng Gao, Jing Xie and Xu-Hui Jin
{"title":"A hydrophilic fully conjugated covalent organic framework for photocatalytic CO2 reduction to CO nearly 100% using pure water†","authors":"Xiaoxiao Yu, Ke Gong, Shuyao Tian, Guangpeng Gao, Jing Xie and Xu-Hui Jin","doi":"10.1039/D2TA10100A","DOIUrl":null,"url":null,"abstract":"<p >Designing stable eco-friendly materials that use abundant H<small><sub>2</sub></small>O as the hydrogen and electron source for photocatalytic conversion of CO<small><sub>2</sub></small> presents a promising route to confronting climate change, but it remains challenging. In this work, we demonstrated that the strategy of converting imine-linkers into 4-carboxyl-quinoline linkages in covalent organic frameworks (COFs) could be used to prepare efficient crystalline porous polymeric photocatalysts for CO<small><sub>2</sub></small> reduction using H<small><sub>2</sub></small>O as the electron donor. In particular, <strong>QL-COF</strong>, featuring hydrophilic 4-carboxyl-quinoline linkages, was found to show improved adsorption of H<small><sub>2</sub></small>O and CO<small><sub>2</sub></small> compared with <strong>LZU1-COF</strong> which was constructed <em>via</em> imine linkages. Theoretical studies indicated that hydrophilic –COOH groups presented strong binding with H<small><sub>2</sub></small>O molecules. Importantly, the pre-adsorbed H<small><sub>2</sub></small>O molecules were found to further enhance the binding of CO<small><sub>2</sub></small> molecules in the pores. The fully conjugated framework of <strong>QL-COF</strong> improved the separation and transfer of photogenerated charge carriers, leading to excellent activity and photostability for photoreduction of CO<small><sub>2</sub></small> with gaseous H<small><sub>2</sub></small>O. Ultimately, <strong>QL-COF</strong> reached a high selectivity of 99.3% for CO generation (156 μmol g<small><sup>?1</sup></small> h<small><sup>?1</sup></small>) under simulated sunlight irradiation.</p>","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":10.7000,"publicationDate":"2023-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2023/ta/d2ta10100a","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Designing stable eco-friendly materials that use abundant H2O as the hydrogen and electron source for photocatalytic conversion of CO2 presents a promising route to confronting climate change, but it remains challenging. In this work, we demonstrated that the strategy of converting imine-linkers into 4-carboxyl-quinoline linkages in covalent organic frameworks (COFs) could be used to prepare efficient crystalline porous polymeric photocatalysts for CO2 reduction using H2O as the electron donor. In particular, QL-COF, featuring hydrophilic 4-carboxyl-quinoline linkages, was found to show improved adsorption of H2O and CO2 compared with LZU1-COF which was constructed via imine linkages. Theoretical studies indicated that hydrophilic –COOH groups presented strong binding with H2O molecules. Importantly, the pre-adsorbed H2O molecules were found to further enhance the binding of CO2 molecules in the pores. The fully conjugated framework of QL-COF improved the separation and transfer of photogenerated charge carriers, leading to excellent activity and photostability for photoreduction of CO2 with gaseous H2O. Ultimately, QL-COF reached a high selectivity of 99.3% for CO generation (156 μmol g?1 h?1) under simulated sunlight irradiation.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.