摘要
采用模板法制备了介孔TiO_2-Al_2O_3载体,以磷酸二氢铵为磷源,硝酸镍为镍源,制备了介孔Ni_2P/TiO_2-Al_2O_3(简称Ni_2P/TA-n,n为Ti与Al的摩尔比,n=1/20,1/10,1/5)催化剂。采用XRD,N2吸附-脱附,SEM,FT-IR,NH_3-TPD和XPS对催化剂进行了表征,并以萘加氢为探针反应,评价了催化剂性能。结果表明,Ni_2P/TA-n(n=1/20,1/10,1/5)催化剂以层状形式存在,钛的引入使得P和Al的化学环境发生改变,可以抑制六配位的Al O6的生成,而且可以减弱载体中四配位Al^(3+)与负载的金属磷化物之间强的相互作用,有利于Ni_2P相的生成。催化剂具有明显的介孔结构,随n的增加,孔容和比表面积先增加后减小。催化剂以中强酸为主,TiO_2的引入降低了Al_2O_3的酸强度。适宜的介孔孔道、酸性和高的Ni_2P相纯度使Ni_2P/TA-n(n=1/20,1/10,1/5)的催化活性和选择性明显高于以溶胶凝胶法制备的TiO_2-Al_2O_3为载体的Ni_2P/TiO_2-Al_2O_3(SG)。介孔Ni_2P/TA-1/10的催化活性和选择性最高,分别达到98.7%和80.5%,催化剂在线使用100 h仍具有活性且选择性没有明显变化。
Mesoporous TiO 2-Al2 O3 carriers were prepared by a template method using ammonium dihydrogen phosphate as the phosphorus source and nickel nitrate as the nickel source. Mesoporous Ni2 P/TiO2-Al2 O3（Ni2 P/TA-n, n is the molar ratio of Ti to Al, n = 1/20, 1/10, 1/5） catalysts were also prepared. The catalysts were characterized by XRD, N2 adsorption-desorption, SEM, FT-IR,NH3-TPD and XPS, and their performance was evaluated via naphthalene hydrogenation. The results show that titanium changes the chemical environment of P and Al, which can prevent the formation of hexa-coordinate AlO 6 and release intensive interaction between P and four coordinate Al^（3＋）. This is favourable for the formation of Ni2 P. The catalysts have obvious mesoporous structure, and their pore volume and specific surface area increase first and then decrease with the increase of n. Ni2 P/TA-n is acidic and the introduction of TiO 2 reduces the acid strength of Al2 O3. Proper pore size, acid strength and high Ni2 P purity result in Ni2 P/TA-n with catalytic activity and decalin selectivity higher than that of Ni2 P/TiO 2-Al2 O3（SG） which was synthesized TiO2-Al2 O3 supported prepared by a sol-gel method. Ni2 P/TA-1/10 has the highest catalytic activity and decalin selectivity, which are 98.7% and 80.5%, respectively. No obvious decrease of catalytic activity and selectivity are found after 100 hours of online time.
作者
刘近
杨丽娜
白金
孙洪宇
李剑
LIU Jin;YANG Li-na;BAI Jin;SUN Hong-yu;LI Jian(Department of Petrochemical Chemistry and Environment,Liaoning Shihna University,Fushtm 113001,China;Liaoning Zhengrun Natural Gas Co.Ltd.,Yingkou 115100,China)
出处
《高校化学工程学报》
EI
CAS
CSCD
北大核心
2018年第4期975-982,共8页
Journal of Chemical Engineering of Chinese Universities
基金
辽宁省高等学校杰出青年学者成长计划(LJQ2015062)
辽宁省科学技术厅项目(20170540585)
辽宁省教育厅项目(L2015296
L2016018)
抚顺市科技计划项目(FSKJHT201376)
关键词
TiO2-Al2O3
NI2P
模板法
加氢
萘
titanium alumina composite
nickel phosphide
template method
hydrogenation
naphthalene
作者简介
刘近（1986-），男，河南周口人，辽宁石油化工大学硕士生。;通讯联系人：李剑，E-mail：yanglnzg@163.com
