Immobilizing Triphenylamine with Photoredox Inert Sr^(2+)Forming Sr-MOF with Controlled Electron Migration for Photocatalytic Oxidation of Thiols to Disulfides  

作　　者：Ying-Xia Wang Fang Zheng Dong-Xia Song Bao-Yue Niu Lu-Qian Deng Xian-Ming Zhang 

机构地区：[1]Key Laboratory of Magnetic Molecules and Magnetic Information Materials(Ministry of Education),Schoolof Chemistry and Materials Science,Shanxi Normal University,Taiyuan,Shanxi 030006,China [2]Key Laboratory of Interface Science and Engineering in Advanced Material(Ministry of Education),College of Chemistry,Taiyuan University of Technology,Taiyuan,Shanxi 030024,China

出　　处：《Chinese Journal of Chemistry》2024年第10期1093-1099,共7页中国化学（英文版）

基　　金：supported by NSFC(22101160);the"1331"Project of Shanxi Province;Research Project Supported by Shanxi Scholarship Council of China(2020-088).

摘　　要：The photocatalytic oxidative coupling of thiols is one of the most popular methods to synthesize the disulfides.Triphenylamine and its derivatives(TPAs)are promising for the above reaction,but suffer from the easy polymerization and difficult separation.To overcome these obstacles while controlling the photogenerated electrons transfer directly to target substrates,herein,we constructed one TPA-based metal-organic framework(MOF),(Me_(2)NH_(2))[Sr(TCBPA)]·DMA·3H_(2)O(1),by direct self-assembly of tris(4′-carboxybiphenyl)amine(H_(3)TCBPA)and photoredox inert strontium ion(Sr^(2+)).DFT calculations revealed that the valence band maximum(VBM)and the conduction band minimum(CBM)are mainly located on TCBPA^(3-),successfully inhibiting the undesirable electron migration to metal nodes.Experimental results indicated that 1 displays superior performance than homogeneous H_(3)TCBPA,which may result from the abundant π…π and C—H…π interactions between the well-arranged TCBPA^(3-)and the build-in electric field between the anionic framework and the Me_(2)NH^(2+).This work highlights that immobilizing TPAs into MOFs is one promising approach to designing heterogeneous photocatalysts for the synthesis of disulfides by oxidative coupling of thiols.

关 键 词：Triphenylamine Metal-organic frameworks STRONTIUM PHOTOOXIDATION THIOLS DISULFIDES 

分 类 号：O62[理学—有机化学]