La-Ni_2P/SBA-15/堇青石整体式催化剂及加氢脱硫性能  

Preparation of La-Ni_2P/SBA-15/cordierite monolithic catalysts and their catalytic performance of hydrodesulfurization

作　　者：吴平易[1,2] 王景艳[2] 兰玲[1] 鞠雅娜[1] 朴佳锐[1] 金辰[1] 胡亚琼[1] 高卓然[1] 季生福[2] 

机构地区：[1]中国石油天然气股份有限公司石油化工研究院,北京100195 [2]北京化工大学化工资源有效利用国家重点实验室,北京100029

出　　处：《工业催化》2014年第4期272-276,共5页Industrial Catalysis

基　　金：国家重点基础研究发展计划(973计划)(2006CB202503)资助项目;中国石油科技创新基金(2010D-5006-0401)资助项目

摘　　要：以介孔分子筛SBA-15为载体,制备一系列不同La含量的La-Ni2P/SBA-15催化剂前驱体,将La-Ni2P/SBA-15前驱体涂覆在预处理的整体式载体堇青石上,在H2气氛程序升温还原,制备不同La含量的La-Ni2P/SBA-15/堇青石整体式催化剂。对合成的催化剂进行X射线衍射和N2吸附-脱附结构表征,并评价对二苯并噻吩的加氢脱硫活性。结果表明,Ni2P存在于所有的La-Ni2P/SBA-15/堇青石整体式催化剂中,且随着La含量的增加,La-Ni2P/SBA-15/堇青石整体式催化剂的比表面积和孔体积均有一定程度的提高,催化活性也提高。对于Ni2P/SBA-15/堇青石整体式催化剂,在300℃和380℃时,二苯并噻吩加氢脱硫转化率仅为27.2%和91.3%;而1.5%La-Ni2P/SBA-15/堇青石催化剂在300℃和380℃时,二苯并噻吩转化率分别为36.8%和96.3%,显示出较好的二苯并噻吩加氢脱硫活性。La-Ni2P/SBA-15/堇青石整体式催化剂在对二苯并噻吩的加氢脱硫过程中,以直接脱硫和加氢脱硫两种脱硫方式同时进行,并且以直接脱硫为主。The catalyst precursors La-Ni2P/SBA-15 were prepared using mesoporous molecular sieve SBA-15 as the carrier. Then a series of La-Ni2P/SBA-15/eordierite monolithic catalysts was prepared by coating the slurry of La-Ni2P/SBA-15 precursors on the pretreated eordierite support, and followed by temperature-programmed reduction in H2 flow. The as-prepared catalysts were characterized by XRD and N2 adsorption-desorption techniques. Their catalytic activity for the hydrodesulfurization （HDS） of dibenzothiophene（DBT） were evaluated. The results showed that Ni2P phase existed in all La-Ni2P/ SBA-15/cordierite monolithic catalysts. The specific surface area, pore volume and the catalytic activity of La-Ni2P/SBA-15/cordierite monolithic catalysts were enhanced with the increase of La contents. At 300 ℃ and 380 ℃, DBT conversion rates over Ni2P/SBA-15/cordierite monolithic catalysts were 27.2% and 91.3%, respectively, while 1.5% La-NizP/SBA-15/cordierite monolithic catalysts exhibited higher HDS activity with DBT conversion rate of 36.8% and 96.3%. The HDS process of DBT over La-Ni2P/ SBA-15/cordierite monolithic catalysts simultaneously had two routes of direct desulfurization（DDS） and hydrogenation（ HYD）, and the main pathway was DDS.

关 键 词：催化化学 La 磷化镍 SBA-15 堇青石 整体式催化剂 直接脱硫 加氢脱硫 

分 类 号：TQ426.6[化学工程] O643.36[理学—物理化学]