载体对镍催化剂催化间二硝基苯加氢制间苯二胺反应性能的影响

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载体对镍催化剂催化间二硝基苯加氢制间苯二胺反应性能的影响

刘迎新^a; 陈吉祥^b; 张继炎^b

^a College of Pharmaceuitcal Science, Zhejiang University of Technology, Hangzhou 310032, China ^b School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

收稿日期:1900-01-01 修回日期:1900-01-01 出版日期:2007-02-28 发布日期:2007-02-28
通讯作者: 刘迎新

Effects of the supports on activity of supported nickel catalysts for hydrogenation of m-dinitrobenzene to m-phenylenediamine

LIU Yingxin^a; CHEN Jixiang^b; ZHANG Jiyan^b

^a College of Pharmaceuitcal Science, Zhejiang University of Technology, Hangzhou 310032, China ^b School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

Received:1900-01-01 Revised:1900-01-01 Online:2007-02-28 Published:2007-02-28
Contact: LIU Yingxin

摘要/Abstract

摘要： The hydrogenation of m-dinitrobenzene to m-phenylenediamine in liquid phase was studied with the nickel catalysts supported on SiO2, TiO2, γ-Al2O3, MgO and diatomite carriers. Based on the experiments of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (TPR), temperature-programmed desorption of hydrogen (H2-TPD) and activity evaluation, the physico-chemical and catalytic properties of the catalysts were investigated. Among the catalysts tested, the SiO2 supported nickel catalyst showed the highest activity and selectivity towards m-phenylenediamine, over which 97.3% m-dinitrobenzene con-version and 95.1% m-phenylenediamine yield were obtained at 373K under hydrogen pressure of 2.6MPa after re-action for 6 h when using ethanol as solvent. Although TiO2 and diatomite supported nickel catalysts also presented high activity, they had lower selectivity towards m-phenylenediamine. As for γ-Al2O3 and MgO supported catalysts were almost inactive for the object reaction. It was shown that both the activity and selectivity of the catalysts were strongly depended on the interaction between nickel and the support. The higher activities of Ni/SiO2, Ni/TiO2 and Ni/diatomite could be attributed to the weaker metal-support interaction, on which Ni species presented as crystal-lized Ni metal particles. On the other hand, there existed strong metal-support interaction in Ni/MgO and Ni/-Al2O3, which causes these catalysts more difficult to be reduced and the availability of Ni active sites de-creased, resulting in their low catalytic activity.

关键词: hydrogenation;m-phenylenediamine;m-dinitrobenzene;supported nickel catalyst;metal-support interaction

Abstract: The hydrogenation of m-dinitrobenzene to m-phenylenediamine in liquid phase was studied with the nickel catalysts supported on SiO2, TiO2, γ-Al2O3, MgO and diatomite carriers. Based on the experiments of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (TPR), temperature-programmed desorption of hydrogen (H2-TPD) and activity evaluation, the physico-chemical and catalytic properties of the catalysts were investigated. Among the catalysts tested, the SiO2 supported nickel catalyst showed the highest activity and selectivity towards m-phenylenediamine, over which 97.3% m-dinitrobenzene con-version and 95.1% m-phenylenediamine yield were obtained at 373K under hydrogen pressure of 2.6MPa after re-action for 6 h when using ethanol as solvent. Although TiO2 and diatomite supported nickel catalysts also presented high activity, they had lower selectivity towards m-phenylenediamine. As for γ-Al2O3 and MgO supported catalysts were almost inactive for the object reaction. It was shown that both the activity and selectivity of the catalysts were strongly depended on the interaction between nickel and the support. The higher activities of Ni/SiO2, Ni/TiO2 and Ni/diatomite could be attributed to the weaker metal-support interaction, on which Ni species presented as crystal-lized Ni metal particles. On the other hand, there existed strong metal-support interaction in Ni/MgO and Ni/-Al2O3, which causes these catalysts more difficult to be reduced and the availability of Ni active sites de-creased, resulting in their low catalytic activity.

Key words: hydrogenation, m-phenylenediamine, m-dinitrobenzene, supported nickel catalyst, metal-support interaction

刘迎新, 陈吉祥, 张继炎. 载体对镍催化剂催化间二硝基苯加氢制间苯二胺反应性能的影响[J]. , DOI: .

LIU ,Yingxin, CHEN ,Jixiang, ZHANG ,Jiyan. Effects of the supports on activity of supported nickel catalysts for hydrogenation of m-dinitrobenzene to m-phenylenediamine[J]. , DOI: .

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