{"title":"Light-driven H2O2 production over redox-active imine-linked covalent organic frameworks","authors":"Songlin Zhang, Jinwen Hu, Wenzhe Shang, Jingya Guo, Xusheng Cheng, Suchan Song, Tianna Liu, Wei Liu, Yantao Shi","doi":"10.1016/j.apmate.2024.100179","DOIUrl":null,"url":null,"abstract":"<div><p>Imine-linked covalent organic frameworks (COFs) provide distinctive prospects for promoting photocatalytic H<sub>2</sub>O<sub>2</sub> production, yet the intricate involvement of imine-derived linkages chemistry under light irradiation remains incompletely elucidated. Here, imine-linked COF-LZU1 demonstrates a visible light-driven H<sub>2</sub>O<sub>2</sub> evolution rate of 387 μmol g<sup>−1</sup> h<sup>−1</sup>, particularly, negligible dependence on the sacrificial agents. By virtue of electron paramagnetic spectroscopy and solid-state nuclear magnetic resonance, we experimentally tracked the structure evolution and identified its autooxidation to Wurster's salt mimics under the photocatalytic conditioning. This finding coincides with the radical anion ·O<sub>2</sub><sup>−</sup> governed reaction pathway and is further rationalized with additional theoretical calculations. This study provides insights into both photophysical/photochemical aspects over the imine-linkage structure.</p></div>","PeriodicalId":7283,"journal":{"name":"Advanced Powder Materials","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2024-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772834X24000101/pdfft?md5=35c3f156dc684b753fcdeddfa4936902&pid=1-s2.0-S2772834X24000101-main.pdf","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Powder Materials","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2772834X24000101","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
Abstract
Imine-linked covalent organic frameworks (COFs) provide distinctive prospects for promoting photocatalytic H2O2 production, yet the intricate involvement of imine-derived linkages chemistry under light irradiation remains incompletely elucidated. Here, imine-linked COF-LZU1 demonstrates a visible light-driven H2O2 evolution rate of 387 μmol g−1 h−1, particularly, negligible dependence on the sacrificial agents. By virtue of electron paramagnetic spectroscopy and solid-state nuclear magnetic resonance, we experimentally tracked the structure evolution and identified its autooxidation to Wurster's salt mimics under the photocatalytic conditioning. This finding coincides with the radical anion ·O2− governed reaction pathway and is further rationalized with additional theoretical calculations. This study provides insights into both photophysical/photochemical aspects over the imine-linkage structure.