Green and selective hydrogenation of aromatic diamines over the nanosheet Ru/g-C_(3)N_(4)-H_(2) catalyst prepared by ultrasonic assisted impregnation-deposition method  

作　　者：Huanhuan Yang Liguo Wang Shuang Xu Yan Cao Peng He Jiaqiang Chen Zheng Zheng Huiquan Li 

机构地区：[1]Key Laboratory of Green Process and Engineering,National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology,Institute of Process Engineering,Chinese Academy of Sciences,Beijing,100190,China [2]Chemical and Biochemical Engineering,Technical University of Denmark,Lyngby 2800 Kgs,Denmark [3]Sino-Danish College,University of Chinese Academy of Sciences,Beijing,100049,China [4]Sino-Danish Center for Education and Research,University of Chinese Academy of Sciences,Beijing,100049,China [5]School of Chemical Engineering,University of Chinese Academy of Sciences,Beijing,100049,China [6]Dalian National Laboratory for Clean Energy,Dalian,116023,China

出　　处：《Green Energy & Environment》2022年第6期1361-1376,共16页绿色能源与环境（英文版）

基　　金：financially supported by the National Nature Science Foundation of China(21576272);“Transformational Technologies for Clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDA 21030600);Science and Technology Service Network Initiative,Chinese Academy of Sciences(KFJ-STS-QYZD-138).

摘　　要：In this study,nanosheet g-C_(3)N_(4)-H_(2) was prepared by thermal exfoliation of bulk g-C_(3)N_(4) under hydrogen.A series of Ru/g-C_(3)N_(4)-H_(2) catalysts with Ru species supported on the nanosheet g-C_(3)N_(4)-H_(2) were synthesized via ultrasonic assisted impregnation-deposition method.Ultrafine Ru nanoparticles(<2 nm)were highly dispersed on nanosheet g-C_(3)N_(4)-H_(2).Strong interaction due to Ru-Nx coordination facilitated the uniform distribution of Ru species.Meanwhile,the involvement of surface basicity derived from abundant nitrogen sites was favourable for enhancing the selective hydrogenation performance of bi-benzene ring,i.e.,almost complete 4,40-diaminodiphenylmethane(MDA)conversion and>99%4,40-diaminodicyclohexylmethane selectivity,corresponding to a reaction activity of 35.7 mol_(MDA) mol_(Ru)^(-1) h^(-1).Moreover,the reaction activity of catalyst in the fifth run was 36.5 mol_(MDA) mol_(Ru)^(-1) h^(-1),which was comparable with that of the fresh one.The computational results showed that g-C_(3)N_(4) as support was favorable for adsorption and dissociation of H_(2) molecules.Moreover,the substrate scope can be successfully expanded to a variety of other aromatic diamines.Therefore,this work provides an efficient and green catalyst system for selective hydrogenation of aromatic diamines.

关 键 词：Nanosheet carbon nitride Ultrafine Ru species Selective hydrogenation Aromatic diamine Alicyclic diamine 

分 类 号：TQ236[化学工程—有机化工]