亢丽娜.Ni/SiO2-Al2O3催化剂在水相加氢体系中的活性及稳定性研究[J].分子催化编辑部,2014,(2):119-125
Ni/SiO2-Al2O3催化剂在水相加氢体系中的活性及稳定性研究
Activity and Stability of Ni/SiO2-Al2O3 catalyst in the aqueous phase hydrogenation system
投稿时间:2014-02-20  修订日期:2014-03-09
DOI:
中文关键词:  氧化硅  氧化铝    水热稳定性  1,4-丁炔二醇
英文关键词:silica  alumina  Nickel  hydrothermal stability  1,4 – butynediol
基金项目:山西省自然科学基金(2013011010-5);国家国际科技合作(2013DFA40460);高等学校博士学科点专项科研基金(20131401120005).
作者单位E-mail
亢丽娜 山西大学化学化工学院 kanglina.923@163.com 
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中文摘要:
      制备了不同Si含量的Ni/SiO2-Al2O3催化剂,通过吡啶-原位傅里叶变换红外(Py-FTIR)、X射线衍射(XRD)、低温N2物理吸附(N2 Physisorption)、H2-程序升温还原(H2-TPR)进行表征,并考察了催化剂在水相1,4-丁炔二醇加氢反应中的活性和稳定性。结果表明:SiO2的引入覆盖了部分γ-Al2O3表面,使暴露的Al3 减少,表现出部分SiO2的表面性质。随Si含量的增加,活性组分Ni与载体之间相互作用减弱,活性组分Ni迁移聚集,催化剂的孔容和孔径减小,Ni/SiO2-Al2O3催化剂初始活性下降。同时,SiO2显著抑制了γ-Al2O3的水合,催化剂的使用稳定性随Si含量的增加而提高,Si含量为3 wt%时,催化剂的初始活性下降幅度较小,而催化剂的水热稳定性显著提高,表现出最佳的反应性能。
英文摘要:
       A series of Ni/SiO2-Al2O3 catalysts with different Si contents were prepared. All the catalysts were characterized by pyridine-in situ Fourier transform infrared (Py-FTIR), X-ray diffraction (XRD), low temperature N2 adsorption (N2 Physisorption), H2-temperature programmed reduction (H2-TPR). The activity and stability in the hydrogenation of aqueous phase 1,4-butynediol was evaluated. The results showed that part of the γ-Al2O3 surface was covered by SiO2, which resulted in the decrease of exposure Al3+. The support exhibited similar properties with SiO2. As the increase of Si, the interaction between the metal Ni and the support was reduced, which caused Ni aggregation, decrease of pore volume and pore diameter, and the decay of the initial activity. Meanwhile, the hydration of γ-Al2O3 was significantly inhibited because of the addition of SiO2. With the raise of Si, the stability of catalyst increased. When the Si content was 3 wt%, the catalyst showed the best performance due to a small decrease of the initial activity and significant increase of the hydrothermal stability.
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