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镍/氧化硅-氧化铝催化剂在含水液相加氢反应中的稳定性研究

发表时间:2017-01-15  浏览量:1490  下载量:350
全部作者: 李海涛,郭江渊,刘琳丽,王志鹏,杨国峰,赵永祥
作者单位: 山西大学精细化学品工程研究中心
摘 要: 分别选用通过在拟薄水铝石中引入SiO2得到的SiO2-Al2O3(SA-1)、在Al2O3中引入SiO2得到的SiO2-Al2O3(SA-2)及Al2O3为载体,采用等体积浸渍法制备Ni负载量为15%的Ni/Al2O3(分别为Ni/SA-1和Ni/SA-2)与Ni/Al2O3催化剂。对比三种催化剂在催化1,4-丁炔二醇高压加氢反应中的使用稳定性,并对使用后的催化剂进行X-射线衍射(X-ray diffraction,XRD)、氮气吸脱附(nitrogen adsorption-desorption)、傅里叶变换红外光谱(Fourier transform infrared spectroscopy,FTIR)、程序升温氧化-质谱联用(temperature programmed oxidation-mass spectroscopy,TPO-MS)表征,研究催化剂的结构、织构变化规律。结果表明,三种催化剂在1,4-丁炔二醇高压加氢反应中均存在不同程度的活性下降,其中Ni/SA-1催化剂不仅具有最高的初始活性,且表现出较其他催化剂更好的使用稳定性。在使用后的催化剂中均存在活性组分镍物种的聚集、表面积炭及孔道堵塞,除此之外,在Ni/Al2O3中还存在载体Al2O3的水合,这些可能是引起催化剂活性下降的主要原因。
关 键 词: 催化化学; 镍/氧化硅-氧化铝;稳定性;液相加氢;1,4-丁炔二醇;1,4-丁二醇
Title: Stability of Ni/silica-alumina catalyst in the hydrogenation of 1,4-butynediol aqueous solution
Author: LI Haitao, GUO Jiangyuan, LIU Linli, WANG Zhipeng, YANG Guofeng, ZHAO Yongxiang
Organization: Research Center for Fine Chemicals Engineering, Shanxi University
Abstract: The SA-1 and SA-2 supports were obtained by introducing silicon oxide into the boehmite and alumina, respectively. The Ni/alumina, Ni/SA-1 and Ni/SA-2 catalysts with 15% Ni loading were prepared by equal volume impregnation method using SA-1, SA-2 and alumina as supports. The stability of catalysts in the catalytic hydrogenation of 1,4-butyndiol was investigated. Also, combined with the X-ray diffraction (XRD), nitrogen adsorption-desorption, Fourier transform infrared spectroscopy (FTIR), temperature programmed oxidation-mass spectroscopy (TPO-MS) methods, the evolution of structure and texture properties of the catalyst was discussed. The results showed that, three kinds of catalysts exhibit different degrees of activity decay in 1,4-butynediol hydrogenation reaction. The Ni/SA-1 catalyst shows not only the highest initial activity, but also better stability than other catalysts. The active component aggregation, surface area carbon and pore blockage exist in the used catalysts. In addition, hydration of alumina also exists in Ni/alumina catalyst. These may be the main causes for the active decay of catalysts.
Key words: catalytic chemistry; Ni/silica-alumina; stability; aqueous phase hydrogenation; 1,4-butynediol; 1,4-butanediol
发表期数: 2017年1月第1期
引用格式: 李海涛,郭江渊,刘琳丽,等. 镍/氧化硅-氧化铝催化剂在含水液相加氢反应中的稳定性研究[J]. 中国科技论文在线精品论文,2017,10(1):76-82.
 
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