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Preparation of Carbon Nanotubes Supported Metal Catalysts and Their Performance in Chloronitrobenzene Hydrogenation Reactions

Author: WangChuang
Tutor: QiuJieShan
School: Dalian University of Technology
Course: Chemical processes
Keywords: Carbon nanotubes Supported catalysts Chloronitrobenzenes Chloroaniline Selective hydrogenation
CLC: TQ246.3
Type: PhD thesis
Year: 2009
Downloads: 835
Quote: 2
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Abstract


The chloronitrobenzenes Hydrogenation chloroanilines is an important class of organic synthesis unit reaction, has a very high industrial value. Over the years, of high performance chloronitrobenzenes hydrogenation catalyst research and development has been one of the hot, highly extensive attention of scholars at home and abroad. This thesis carbon nanotubes (CNTs) supported Pt bimetallic PtM (M = Fe, Co, Ni, Cu) the hydrogenation catalytic properties of the catalyst chloronitrobenzenes analysis of the impact of the Pt / CNTs and PtM / CNTs catalytic performance of the key factors. Preparation of low Pd / CNTs catalyst chloronitrobenzene hydrogenation selectivity composite bimetallic catalyst Pd / SnO 2 / CNTs, the choice of the catalyst chloronitrobenzene the hydrogenation catalytic properties investigated the main parameters that affect the catalytic activity and selectivity, and analyzes the main reason for the selectivity of the catalyst than Pd / CNTs. Precious Metal Resources are scarce, expensive, prepared carbon nanotubes load transition of non-precious metals Ni, Co catalyst preparation conditions on the catalytic hydrogenation activity chloronitrobenzenes. In addition, the preliminary study feasibility of the select load Ag catalyst in carbon nanotubes chloronitrobenzenes application in the hydrogenation reaction. The research results show that the bimetallic catalysts Pt / CNTs PtM / CNTs with good o-chloronitrobenzene Selective Hydrogenation performance. The activation temperature to selective hydrogenation catalytic performance of Pt / CNTs catalyst particle size and chloronitrobenzenes significant impact. With the activation temperature rise, Pt catalyst average particle size gradually increases catalytic o-chloronitrobenzene hydrogenation activity first increased and then decreased 400 ° C activation Pt / CNTs catalyst highest catalytic activity. The the bimetallic PtNi / CNTs catalyst impregnation order their catalytic properties greater impact: co-impregnation the prepared Pt-Ni/CNTs catalyst, the catalytic activity decreased gradually with the increase of Ni content; first impregnated Ni precursor and then restore after impregnated Pt precursor reduction with Pt / Ni / CNTs catalyst activity higher than single-metal Pt / CNTs catalyst the Pt Ni content of 0.15% / Ni / CNTs catalyst showed the highest activity. Prepared Pt / Fe / CNTs, Pt / Co / CNTs, Pt / Cu / CNTs catalyst has high chloronitrobenzene hydrogenation catalytic activity. Pd / SnO 2 / CNTs can effectively inhibit the dechlorination of the o-CAN, under conditions to maintain a high catalytic activity, to improve the selectivity of the target product. Sn / Pd molar ratio affect Pd / SnO the 2 / CNTs catalytic properties of parameters. Sn / Pd = 11, Pd / SnO 2 / CNTs catalyst has the best catalytic activity, the reaction at atmospheric pressure of 60 ° C for 60min, 96% of o-CNB conversion was impregnated with the same load Preparation of 2.4% Pd / CNTs considerable catalytic activity. When o-CNB reacted completely finished, Pd / SnO 2 / CNTs catalyst o-CAN selectivity can reach 95%, while only 22 o-CAN selectivity of the Pd / CNTs catalyst %. SnO 2 modulation effects Pd / SnO 2 / CNTs catalyst selectivity main reason for the high. Ni / CNTs catalyst showed higher chloronitrobenzene hydrogenation activity. By comparing a dipping method, deposition-precipitation of an aqueous solution, and a polyol solvent deposition precipitation method, and found that the method and conditions of preparation of the catalyst performance of its catalytic hydrogenation greater impact. Polyol solvent deposition prepared by precipitation of Ni / CNTs catalyst highest catalytic activity. The type of solvent and the precipitation temperature affect the the polyol solvent deposition composition of precipitation the prepared NiCNTs catalyst particle size and o-CNB hydrogenation performance parameters. Glycol as solvent precipitation temperature prepared Ni / CNTs catalyst Ni content similar; 120 ℃ and 160 ℃ prepared Ni / CNTs catalyst average particle size of the smallest, 5.1nm and 5.7 nm, 80 ° C Preparation of Ni / CNTs the larger the average particle diameter of the catalyst is 10.7 nm; 80 ℃ prepared Ni / CNTs as - prepared Catalyst highest activity to react at 140 ℃, 2 MPa for 30 min, O-CNB conversion rate reached 91%, the choice of the O-CAN was 97%. Preparation of Ni / CNTs catalyst, Ni content as the precipitation temperature rise increased glycerol deposition-precipitation solvent, but were lower than the same temperature for the ethylene glycol solvent to prepare a catalyst of Ni, Ni / CNTs content; Ni / CNTs The catalytic activity of the catalyst with the precipitation temperature rise is increased, 160 ° C Preparation of Ni / CNTs catalyst highest catalytic activity, O-CNB conversion was 72%, the O-CAN selectivity of 97%. The catalytic performance of Ni / CNTs better than the Ni / AC, possible due to the interaction between the carrier and the metal is different, and carbon nanotubes unique pore structure conducive to the reaction of the mass transfer. Ag / CNTs catalyst has certain chloronitrobenzene hydrogenation catalytic activity. Ag / CNTs catalyst can be prepared by the catalytic activity by deposition-precipitation method, the pH of the solution in the preparation process, the AgNO 3 concentration and precipitation temperature affect the key factors of the Ag / CNTs catalytic performance.

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CLC: > Industrial Technology > Chemical Industry > Basic Organic Chemistry Industry > The production of aromatic compounds > Aromatic nitrogen compounds > Aromatic amines and their derivatives
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