| Ni/Fe物质的量的比对Ni-Fe催化剂表面性质和二硝基甲苯加氢活性的影响 |
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| 引用本文： | 郝志强,于智慧,李忠.Ni/Fe物质的量的比对Ni-Fe催化剂表面性质和二硝基甲苯加氢活性的影响[J].无机化学学报,2015,31(8):1571-1580. |
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| 作者姓名： | 郝志强 于智慧 李忠 |
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| 作者单位： | 太原理工大学, 煤科学与技术教育部与山西省重点实验室, 太原 030024,赛鼎工程有限公司, 太原 030024,太原理工大学, 煤科学与技术教育部与山西省重点实验室, 太原 030024 |
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| 基金项目： | 国家"973"计划(No.2012CB723105)资助项目。 |
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| 摘 要： | 采用Fe粉置换氯化镍溶液中的Ni2+制备了Ni-Fe催化剂,并应用于催化二硝基甲苯加氢合成甲苯二胺的反应中。运用XRD、低温氮吸附-脱附、H2-TPD、XPS和TEM等技术手段对不同Ni/Fe物质的量的比(nNi/nFe)下催化剂进行了表征。结果表明,nNi/nFe对Ni-Fe催化剂表面性质影响显著。当nNi/nFe为1:4时,Fe抑制Ni氧化的作用达到最大,Ni-Fe催化剂化学氢吸附量和活性物种Ni的分散度分别达到了0.16 mmol·g-1和23%,催化剂性能得到较大的提升。在优化的催化剂制备条件下,DNT(二硝基甲苯)的转化率和TDA(甲苯二胺)的选择性分别达到了~100%和99%。另外,对Ni-Zn漆原镍(Urushibara Ni)催化剂和Ni-Fe催化剂催化DNT加氢反应进程进行了研究,发现它们有相同的加氢中间产物,但反应不同阶段的催化速率存在差异。
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| 关 键 词： | Ni-Fe催化剂 二硝基甲苯 甲苯二胺 催化加氢 |
| 收稿时间： | 2015/4/12 0:00:00 |
| 修稿时间： | 2015/5/21 0:00:00 |
Influence of Ni/Fe Molar Ratio on Surface Properties of Ni-Fe Catalysts and Hydrogenation Performance of Dinitrotoluene |
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| HAO Zhi-Qiang,YU Zhi-Hui and LI Zhong.Influence of Ni/Fe Molar Ratio on Surface Properties of Ni-Fe Catalysts and Hydrogenation Performance of Dinitrotoluene[J].Chinese Journal of Inorganic Chemistry,2015,31(8):1571-1580. |
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| Authors: | HAO Zhi-Qiang YU Zhi-Hui and LI Zhong |
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| Institution: | Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China,Sedin Engineering Company Limited, Taiyuan 030024, China and Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, China |
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| Abstract: | Ni-Fe catalysts were prepared via the replacement reaction of NiCl2 by Fe and used for the selective hydrogenation of dinitrotoluene (DNT) in liquid phase. The influences of Ni/Fe molar ratio (nNi/nFe) on the surface properties and catalytic performance of Ni-Fe catalysts were investigated. The characterization results from XRD, Low temperature nitrogen adsorption -desorption, H2-TPD, XPS and TEM show that nNi/nFe has a significant effect on the surface properties of Ni-Fe catalysts. When nNi/nFe is 1:4, the effect of Fe inhibition on the oxidation of nickel is more apparent, the chemical adsorption of hydrogen is 0.16 mmol·g-1 and the dispersion of active species Ni achieves 23%. The performance of Ni-Fe catalysts is greatly improved. Under the optimized catalysts preparation conditions, the conversion of DNT (dinitrotoluene) and the selectivity of TDA (toluenediamine) could reach~100% and 99%, respectively. In addition, Ni-Zn Urushibara nickel catalysts and Ni-Fe catalysts have~the same catalytic hydrogenation~pathway but different catalytic reaction rate in a different reaction stages. |
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| Keywords: | Ni-Fe catalyst dinitrotoluene toluenediamine catalytic hydrogenation |
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