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The ethylbenzene hydrogenation over Ni-H_3PW_(12)O_(40)/SiO_2 in the presence of thiophene

机译:Ni-H_3PW_(12)O_(40)/ SiO_2在噻吩存在下的乙苯加氢反应

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摘要

Ni-HPW/SiO_2 catalysts with H_3PW_(12)O_(40) (HPW) loading in the range of 0.1-8% were prepared by a modified sol-gel method. The as-prepared catalysts with bimodal pore distribution not only possess relatively large pore and surface area, but exhibit high activity for ethylbenzene hydrogenation even in the presence of thiophene up to 640 ppm. It is evident that nickel oxide particles are small and well-dispersed on the surface of these catalysts from X-ray powder diffraction (XRD), scanning electron microscopy (SEM) and transmission electron microscopy (TEM) characterization. The results of temperature-programmed reduction of hydrogen (H_2-TPR), temperature-programmed desorption of hydrogen and ammonia (H_2 and NH_3-TPD) also strongly suggest the interaction between Ni component and HPW takes place, and consequently results in remarkable H_2 spillover and considerable increase of acidic site concentration of Ni-HPW/SiO_2 catalysts. Further, the results of Fourier transform infrared spectroscopy (FT-IR) with pyridine adsorption also show that most of the acid sites are related to Lewis acid and the metal Ni species on the surface of catalysts are therefore prone to be electron-deficient. It is confirmed that HPW plays a critical role in the improvement of sulfur resistance for Ni-based catalysts.
机译:采用改进的溶胶-凝胶法制备了H_3PW_(12)O_(40)(HPW)负载量为0.1-8%的Ni-HPW / SiO_2催化剂。所制备的具有双峰孔分布的催化剂不仅具有相对较大的孔和表面积,而且即使在存在高达640 ppm的噻吩的情况下,也表现出对乙苯加氢的高活性。通过X射线粉末衍射(XRD),扫描电子显微镜(SEM)和透射电子显微镜(TEM)表征,显然氧化镍颗粒很小并且很好地分散在这些催化剂的表面上。程序升温还原氢气(H_2-TPR),程序升温还原氢气和氨气(H_2和NH_3-TPD)的结果也强烈表明Ni组分与HPW之间发生了相互作用,因此导致显着的H_2溢出Ni-HPW / SiO_2催化剂酸性位点浓度的显着增加。此外,具有吡啶吸附的傅立叶变换红外光谱法(FT-IR)的结果还表明,大多数酸位与路易斯酸有关,因此催化剂表面上的金属Ni种类倾向于缺乏电子。证实HPW在改善Ni基催化剂的抗硫性中起关键作用。

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  • 来源
    《Fuel》 |2013年第2期|547-552|共6页
  • 作者单位

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

    National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory for Physical Chemistry of the Solid Surfaces,College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Ni-based catalyst; heteropoly acid; aromatics hydrogenation; sulfur resistance;

    机译:镍基催化剂;杂多酸芳烃加氢耐硫性;

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