High performance of a cobalt-nitrogen complex for the reduction and reductive coupling of nitro compounds into amines and their derivatives

被引:468
作者
Zhou, Peng [1 ]
Jiang, Liang [1 ]
Wang, Fan [1 ]
Deng, Kejian [1 ]
Lv, Kangle [1 ]
Zhang, Zehui [1 ]
机构
[1] South Cent Univ Nationalities, Key Lab Catalysis & Mat Sci, Minist Educ, Wuhan 430074, Peoples R China
基金
中国国家自然科学基金;
关键词
CATALYTIC TRANSFER HYDROGENATION; OXYGEN REDUCTION; CHEMOSELECTIVE HYDROGENATION; ROOM-TEMPERATURE; ACTIVE-SITES; NITROARENES; ELECTROCATALYST; NITROBENZENE; EFFICIENT; POLYMER;
D O I
10.1126/sciadv.1601945
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Replacement of precious noble metal catalysts with low-cost, non-noble heterogeneous catalysts for chemoselective reduction and reductive coupling of nitro compounds holds tremendous promise for the clean synthesis of nitrogencontaining chemicals. We report a robust cobalt-nitrogen/carbon (Co-N-x/C-800-AT) catalyst for the reduction and reductive coupling of nitro compounds into amines and their derivates. The Co-N-x/C-800-AT catalyst was prepared by the pyrolysis of cobalt phthalocyanine-silica colloid composites and the subsequent removal of silica template and cobalt nanoparticles. The Co-N-x/C-800-AT catalyst showed extremely high activity, chemoselectivity, and stability toward the reduction of nitro compounds with H2, affording full conversion and > 97% selectivity in water after 1.5 hours at 110 degrees C and under a H2 pressure of 3.5 bar for all cases. The hydrogenation of nitrobenzene over the Co-N-x/C-800-AT catalyst can even be smoothly performed under very mild conditions (40 degrees C and a H2 pressure of 1 bar) with an aniline yield of 98.7%. Moreover, the Co-N-x/C-800-AT catalyst has high activity toward the transfer hydrogenation of nitrobenzene into aniline and the reductive coupling of nitrobenzene into other derivates with high yields. These processes were carried out in an environmentally friendly manner without base and ligands.
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页数:10
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