Enhanced tandem hydrogenation of nitroaromatics to alicyclic amines via Pt-Ru synergistic catalysis

被引:0
|
作者
Wu, Jiale [1 ,2 ,3 ]
Zhang, Jiajun [1 ]
Wang, Liguo [1 ,2 ,3 ]
Han, Ziqiang [1 ]
Hui, Xiang [1 ]
Cao, Yan [1 ]
Shi, Jianhui [1 ]
Xu, Shuang [1 ]
He, Peng [1 ]
Li, Huiquan [1 ,2 ,3 ,4 ]
机构
[1] Chinese Acad Sci, Inst Proc Engn, Natl Engn Res Ctr Green Recycling Strateg Met Reso, CAS Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
[2] Univ Chinese Acad Sci, Sino Danish Coll, Beijing 100049, Peoples R China
[3] Univ Chinese Acad Sci, Sino Danish Ctr Educ & Res, Beijing 100049, Peoples R China
[4] Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
Nitroaromatics; Tandem hydrogenation; Alicyclic amines; Hydrogen spillover; Bimetal catalysts; SITU INFRARED-SPECTROSCOPY; CHEMOSELECTIVE HYDROGENATION; MESOPOROUS CARBON; CYCLOHEXYLAMINE; NITROBENZENE; ASSIGNMENTS; ANILINE; INSIGHT;
D O I
10.1016/j.cej.2024.151083
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Green production of alicyclic amines is highly desirable but of great challenges. Herein, an efficient one-pot synthesis of alicyclic amines from nitroaromatics was realized with a Pt-Ru bimetallic catalyst. 0.5 %Pt-2.5 % Ru supported on an air-exfoliated C3N4 nanosheet achieved 100.0 % conversion of nitrobenzene (NB) with 98.9 % selectivity of cyclohexylamine (CHA) under mild conditions of 80 degrees C and 1 MPa, attaining a yield rate for alicyclic amine of 357.9 mmol/gmetal & sdot;h. Our study has shown hydrogenation of nitro group and aromatic ring took place in sequence over Pt and Ru in a tandem manner due to the highly selective adsorption. During the hydrogenation, the homolytic dissociation of H2 occurred on the bimetal sites and the inter-site hydrogen spillover between the bimetal played a crucial role. C3N4 nanosheet as the support not only gave rise to the uniform dispersion of metal nanoparticles, but was crucial in curbing the unnecessary adsorption of intermediate aromatic amines. Our study has also demonstrated the good stability and wide applicability of the Pt-Ru/C3N4-air catalyst for the hydrogenation of various nitroaromatic derivatives.
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页数:13
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