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Room-temperature hydrogenation of halogenated nitrobenzenes over metal-organic-framework-derived ultra-dispersed Ni stabilized by N-doped carbon nanoneedles

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Frontiers of Chemical Science and Engineering 2022年第12期16卷 1782-1792页

作者： Yuemin Lin Yuanyuan Zhang Renfeng Nie Kai Zhou Yao Ma Mingjie Liu Dan Lu Zongbi Bao Qiwei Yang Yiwen Yang Qilong Ren Zhiguo Zhang Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China School of Chemical Engineering Henan Center for Outstanding Overseas ScientistsZhengzhou UniversityZhengzhou 450001China Institute of Zhejiang University—Quzhou Quzhou 324000China

Ultra-dispersed Ni nanoparticles(7.5 nm)on nitrogen-doped carbon nanoneedles(Ni@NCNs)were prepared by simple pyrolysis of Ni-based metal–organic-framework for selective hydrogenation of halogenated nitrobenzenes to corresponding *** different crystallization methods(stirring and static)were compared and the optimal pyrolysis temperature was ***@NCNs were systematically characterized by wide analytical *** the hydrogenation of p-chloronitrobenzene,Ni@NCNs-600(pyrolyzed at 600°C)exhibited extraordinarily high performance with 77.9 h^(–1)catalytic productivity and>99%p-chloroaniline selectivity at full p-chloronitrobenzene conversion under mild conditions(90°C,1.5 MPa H2),showing obvious superiority compared with reported Ni-based ***,the reaction smoothly proceeded at room temperature with full conversion and>99%***,Ni@NCNs-600 afforded good tolerance to various nitroarenes substituted by sensitive groups(halogen,nitrile,keto,carboxylic,etc.),and could be easily recycled by magnetic separation and reused for 5 times without *** adsorption tests showed that the preferential adsorption of–NO2 on the catalyst can restrain the dehalogenation of p-chloronitrobenzene,thus achieving high p-chloroaniline *** the high activity can be attributed to high Ni dispersion,special morphology,and rich pore structure of the catalyst.

关键词： halogenated nitrobenzenes room-temperature hydrogenation Ni nanoparticles nitrogen-doped carbon nanoneedles metal–organic-framework

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The promoting role of minor amount of water in solvent-free hydrogenation of halogenated nitrobenzenes

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Chinese Chemical Letters 2014年第2期25卷 205-208页

作者： Jing-Hui Lyu Xiao-Bo He Chun-Shan Lu Lei Ma Qun-Feng Zhang Feng Feng Xiao-Nian Li Jian-Guo Wang Institute of Industrial Catalysis College of Chemical Engineering and Materials ScienceZhejiang University of Technology

This study shows that minor amount of water plays a very important role in solvent-free hydrogenation of halogenated nitrobenzenes. For dried sponge Pd, the reaction cannot occur in the absence of water. For Pd/C catalyst, minor amount of water reduces the induction time, increases the reaction rate and reaction TOFs. Water might enhance the diffusion, adsorption and dissociation of H2 on Pd catalysts.

关键词： halogenated nitrobenzenes Solvent Free Water Hydrogenation

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