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2,4-二硝基甲苯无溶剂加氢表观动力学研究

发表时间:2010-03-15  浏览量:1757  下载量:676
全部作者: 孔令启,李春欣,葛纪军,曹传波,张国平
作者单位: 青岛科技大学计算机与化工研究所;甘肃银光化工集团;青岛银科恒远化工过程信息技术有限公司
摘 要: 在自行设计的反应装置中以骨架镍为催化剂,在无溶剂环境下2,4-二硝基甲苯(2,4-dinitrotoluene, DNT)加氢合成2,4-甲苯二胺(2,4-toluene diamine, TDA)。考察了温度为100~140℃、氢气压力为1.0~3.0 MPa、催化剂质量浓度为0.03%~2.00%、TDA质量浓度为30%~70%情况下对反应的影响。研究表明:反应速率与氢气压力成正比;DNT加氢反应在高浓度区(DNT浓度大于7.14 mol·m-3)为吸附脱附控制,催化剂浓度与反应速率成正比,DNT浓度对反应速率无影响;而在低浓度区(DNT浓度小于7.14 mol·m-3),该反应为界面反应控制,催化剂浓度在一定范围内对反应速率影响不大,DNT浓度对反应速率影响为1级。DNT低浓度区和高浓度区的活化能分别为17.62,15.67 kJ·mol-1,表明无溶剂条件下催化剂可大幅降低反应活化能而使反应更快进行;在实验条件范围内,TDA含量对反应速率基本无影响;并由此得到该反应的表观反应动力学。工程数据验证了模型的正确性,研究结论可为DNT无溶剂加氢工艺过程和加氢反应器设计提供理论指导。
关 键 词: 化学反应工程;动力学模型;催化加氢;2,4-二硝基甲苯;无溶剂
Title: Macro-kinetics studies on non-solvent catalytic hydrogenation of 2,4-diaminotoluene
Author: KONG Lingqi, LI Chunxin, GE Jijun, CAO Chuanbo, ZHANG Guoping
Organization: Research Center of Computer and Chemical Engineering, Qingdao University of Science and Technolog;Gansu Yinguang Chemmical Industry Group Co., Ltd.;Qingdao Yinke Hengyuan Process Technology Co.,Ltd.
Abstract: The process and kinetics of liquid phase hydrogenation of 2,4-dinitrotoluene (DNT) to 2,4-toluene diamine (TDA) with no solvent were observed with a self-designed device at 100~140℃, 1.0~3.0 MPa, Ni catalyst concentration (CNi) of 0.03%~2.00% by weight,and content of TDA 30%~70% by weight. Experimental data showed that the reaction has different properties in the low DNT content region (CDNT <7.14 mol·m-3, LDCR) from that in the high DNT content region (CDNT>7.14 mol·m-3, HDCR). In HDCR, the reaction was controlled by adsorptive process, and CNi was in direct proportion to the reaction rate while CDNT had almost no effect on it. In LDCR, the reaction was controlled by interface reaction process, and CNi had no effect on the reaction rate in a certain range while CDNT was in direct proportion to it. In both regions the reaction rate is about in direct proportion to hydrogen pressure. The apparent activation energies of the reaction in both regions were also obtained, 17.62 and 15.67 kJ·mol-1 respectively, which reveald that the reaction was more easily occurred than that in the solvent environment. The content of TDA had no effect on the reaction rate. The macro-kinetics was obtained through data fitting. An excellent agreement between the model predictions and the experimental data was observed, which showed that the study result could provide theoretical direction to non-solvent catalytic hydrogenation of DNT and hydrogenation reactor design.
Key words: chemical reaction engineering;kinetic model; catalystic hydrogenation; 2,4-dinitrotoluene; non-solvent
发表期数: 2010年3月第5期
引用格式: 孔令启,李春欣,葛纪军,等. 2,4-二硝基甲苯无溶剂加氢表观动力学研究[J]. 中国科技论文在线精品论文,2010,3(5):512-519.
 
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