Improved catalytic performance of acid-activated sepiolite supported nickel and potassium bimetallic catalysts for liquid phase hydrogenation of 1,6-hexanedinitrile

Yang Lv , Fang Hao , Pingle Liu , Shaofeng Xiong , He’an Luo
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引用次数: 20

Abstract

Different inorganic acids were used to activate sepiolite, and the acid-activated sepiolites supported nickel and potassium bimetallic catalysts were prepared. Nitrogen adsorption-desorption, hydrogen chemisorption, ammonia temperature programmed desorption (NH3-TPD), temperature programmed reduction (TPR), powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier Transform Infrared Spectroscopy (FTIR) and energy dispersive X-ray (EDX) were used to characterize the catalysts. The catalytic performance of the acid-activated sepiolite supported K-Ni bimetallic catalysts were investigated in 1,6-hexanedinitrile (HDN) hydrogenation in liquid phase. It was revealed that the potassium could increase the alkalinity of the catalyst with the aim of inhibiting the formation of the 1-azacycloheptane (ACH). And the addition of potassium reduces the particle size of nickel and improves its dispersion. Compared with hydrochloric acid and sulfuric acid, nitric acid treatment increases more silanol groups (SiOH) on the sepiolite surface, which is helpful to nickel particles adsorption and dispersion. Nitric acid activated sepiolite supported nickel and potassium bimetallic catalysts (K-Ni/NASEP) present the best catalytic performance, the conversion of HDN comes up to 92.0% under moderate conditions of lower temperature and pressure, the selectivity to 6-aminocapronitrile (ACN) and 1,6-hexanediamine (HDA) is up to 95.2%.

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改善酸活化海泡石负载镍钾双金属催化剂对1,6-己二腈液相加氢的催化性能
采用不同的无机酸对海泡石进行活化,制备了酸活化海泡石负载型镍钾双金属催化剂。采用氮气吸附-解吸、氢气化学吸附、氨程序升温解吸(NH3-TPD)、程序升温还原(TPR)、粉末x射线衍射(XRD)、扫描电镜(SEM)、透射电镜(TEM)、傅里叶变换红外光谱(FTIR)和能量色散x射线(EDX)对催化剂进行了表征。研究了酸活化海泡石负载的K-Ni双金属催化剂对1,6-己二腈(HDN)液相加氢的催化性能。结果表明,钾可以提高催化剂的碱度,从而抑制1-氮杂环庚烷(ACH)的生成。钾的加入降低了镍的粒径,改善了镍的分散性。与盐酸和硫酸处理相比,硝酸处理增加了海泡石表面更多的硅醇基团(SiOH),有利于镍颗粒的吸附和分散。硝酸活化海泡石负载的镍钾双金属催化剂(K-Ni/NASEP)表现出最好的催化性能,在较低的温度和压力下,HDN的转化率可达92.0%,对6-氨基己二腈(ACN)和1,6-己二胺(HDA)的选择性可达95.2%。
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期刊介绍: The Journal of Molecular Catalysis A: Chemical publishes original, rigorous, and scholarly full papers that examine the molecular and atomic aspects of catalytic activation and reaction mechanisms in homogeneous catalysis, heterogeneous catalysis (including supported organometallic catalysis), and computational catalysis.
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