Zwitterionic cellular polymer enabled reductive fixation of CO_(2) for N-methylation of amines  

作　　者：Wenfeng Zhao Hu Li Hang Cong Hongguo Wu Ping Zhu Song Yang 

机构地区：[1]National Key Laboratory of Green Pesticide,Key Laboratory of Green Pesticide and Agricultural Bioengineering(Ministry of Education),State-Local Joint Engineering Lab for Comprehensive Utilization of Biomass,Center for R&D of Fine Chemicals,Guizhou University,Guiyang 550025,China [2]Key Laboratory of Macrocyclic and Supramolecular Chemistry of Guizhou Province,School of Chemistry and Chemical Engineering,Guizhou University Guiyang 550025,China [3]Centre for Catalysis and Sustainable Chemistry,Department of Chemistry,Kemitorvet Building 207,Technical University of Denmark,Lyngby DK-2800,Denmark

出　　处：《Green Synthesis and Catalysis》2023年第4期342-349,共8页绿色合成与催化（英文）

基　　金：This study was financially supported by the Guizhou Provincial S&T Project(Nos.ZK[2022]011 and 2018[4007]);the National Natural Science Foundation of China(No.21908033);the Fok Ying-Tong Education Foundation(161030).

摘　　要：Using heterogeneous catalysts to promote the construction of the C–N bond between amines and CO_(2) under mild conditions is a challenge yet.Herein,we synthesized a novel zwitterionic polymer(PDDC)with a cellular structure via self-complexation of copolymer bearing both quaternary ammonium cation and carboxylate anion.PDDC was employed as a recyclable catalyst for N-methylation of atmospheric CO_(2) and various amines with hydrosilane as a reductant,affording more than 17 N-methylamines in good to excellent yields(up to 99%)under mild conditions.The behavior of PDDC in the reaction medium was disclosed by using a dynamic light scattering study,revealing that the decreased hydraulic radius of particle size contributes to exposing more active sites and increasing reaction activity.Utilizing a series of designed experiments and density functional theory calculations uncovered the crucial role of the prepared zwitterionic polymer during the reaction procedure of CO_(2) conversion.

关 键 词：CO_(2)utilization Porous polymer Zwitterionic ion N-METHYLATION Heterogeneous catalysis 

分 类 号：O62[理学—有机化学]