Liquid phase hydrogenation of adiponitrile over acid-activated sepiolite supported K–La–Ni trimetallic catalysts
Liquid phase hydrogenation of adiponitrile over acid-activated sepiolite supported K–La–Ni trimetallic catalysts
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DOI：
10.1007/s11144-016-1061-2
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发表时间：
2016-08
期刊：
影响因子：
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通讯作者：
Yang Lv;F. Hao;Pingle Liu;Shaofeng Xiong;He'an Luo
中科院分区：
文献类型：
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作者：
Yang Lv;F. Hao;Pingle Liu;Shaofeng Xiong;He'an Luo
制备了酸活化海泡石负载的K-La-Ni三金属催化剂，并将其用于己二腈(ADN)的液相加氢反应。用稀盐酸溶液处理海泡石制得海泡石，采用浸渍法制备了海泡石负载的K-La-Ni三金属催化剂，并用氮气吸附-脱附、程序升温还原、氢气化学吸附、粉末X射线衍射、透射电子显微镜、扫描电子显微镜、傅立叶变换红外光谱和能量色散X射线对其进行了表征。结果表明，钾可以通过中和催化剂上的一些酸性中心来抑制1-氮杂环庚烷副产物的生成，而钾和镧可以有效地减小镍颗粒的尺寸，改善其分散性。海泡石经盐酸处理后，表面硅醇基(Si-OH)增多，有利于镍粒子的吸附和分散。ASEP负载K-La-Ni三金属催化剂(K-La-Ni/AsEP)在温和的反应条件下(373K和2.0 Mpa)表现出较好的催化性能，ADN转化率达到90.03%，6-氨基异氰酸酯和六亚甲二胺的选择性达到90.22%。
Acid-activated sepiolite (ASEP) supported K–La–Ni trimetallic catalysts were prepared and tested in the liquid phase hydrogenation of adiponitrile (ADN). The sepiolite was treated with dilute hydrochloric acid solution to obtain ASEP, ASEP supported K–La–Ni trimetallic catalysts were prepared by the incipient impregnation method and characterized by nitrogen adsorption–desorption, temperature programmed reduction, hydrogen chemisorption, powder X-ray diffraction, transmission electron microscopy, scanning electron microscopy, Fourier transform infrared spectroscopy and energy dispersive X-ray. It was revealed that potassium could inhibit the formation of the 1-azacycloheptane by-product by neutralizing some acid sites on the catalyst, and the potassium and lanthanum could efficiently reduce nickel particles size and improve its dispersion. Sepiolite treated with hydrochloric acid increases the number of silanol groups (Si–OH) on the sepiolite surface, which is helpful to nickel particles adsorption and dispersion. ASEP supported K–La–Ni trimetallic catalysts (K–La–Ni/ASEP) present better catalytic performance under mild reaction conditions of 373 K and 2.0 MPa, the ADN conversion reaches to 90.03 %, the selectivity to 6-aminocapronitrile and hexamethylenediamine is up to 90.22 %.