Na_2O及其引入顺序对Ni-Mo/MCM-41催化剂加氢脱硫性能的影响  

INFLUENCE OF Na_2O AND ITS INTRODUCTION SEQUENCE ON THE HYDRODESULFURIZATION PERFORMANCE OF Ni-Mo/MCM-41

作　　者：李金亮[1] 李翔[1,2] 王安杰[1,2] 果崇申[1] 

机构地区：[1]大连理工大学化工学院,辽宁大连116023 [2]辽宁省高校石油化工技术与装备重点实验室,辽宁大连116023

出　　处：《石油学报（石油加工）》2010年第6期859-864,共6页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金重点基金(20333030);国家自然科学基金青年基金(20503003);国家自然科学基金(20773020);辽宁省中青年学科带头人和教育部博士点专项基金项目资助

摘　　要：采用不同顺序将Na2O引入到NiMo/MCM-41催化剂前驱体中,并以质量分数0.8%的二苯并噻吩(DBT)的十氢萘溶液作模型化合物,考察了催化剂的加氢脱硫(HDS)催化性能。结果表明,引入Na2O促进了NiMo/MCM-41催化剂前驱体中-βNiMoO4物种的生成,不利于活性组分的分散,同时还抑制了其还原。分步浸渍法引入Na2O影响了催化剂中Mo物种的配位状态。Na2O引入顺序对NiMo/MCM-41催化剂HDS催化活性有较大影响。共浸渍法引入Na2O时,同时抑制了催化剂的加氢反应路径(HYD)和直接脱硫反应路径(DDS)催化活性,因此其HDS催化活性最低。与共浸渍和在活性组分之后引入Na2O相比,在活性组分之前引入Na2O对催化剂的HYD催化活性影响最小,但DDS催化活性显著增加,提高了总的HDS催化活性。通过控制碱金属氧化物的引入顺序,可以调变催化剂活性和选择性,是一种对硫化物催化剂有效的改性方法。Na2O was introduced to NiMo/MCM-41 catalyst precursor by different sequences,and the hydrodesulfurization（HDS） performances of the prepared catalysts were studied by using a model fuel of decalin solution containing 0.8% DBT.The results indicated that the introduction of Na2O not only facilitated the formation of β-NiMoO4,leading to decreased dispersion of active species,but also suppressed the reducibility of NiMo/MCM-41 precursor.The coordination states of Mo species were affected by Na2O introduced by the consecutive impregnation methods.The HDS activity of NiMo/MCM-41 was strongly affected by the Na2O introduction sequence.For the catalyst in which Na2O was introduced by a co-impregnation method,both the activities of the hydrogenation pathway（HYD） and direct desulfurization pathway（DDS） were suppressed,resulting in a decrease in the overall HDS activity.Compared with the co-impregnation and the introduction of Na2O after NiMo active components,the addition of Na2O before the deposition of these active components showed much less influence on the HYD activity,but significantly enhanced DDS activity of NiMo/MCM-41,thus an improvement in the overall HDS activity was observed.Both the activity and selectivity of the sulfide catalysts can be modified by adapting a proper addition sequence of the alkali-metal oxides,which is an effective way for the modification of HDS catalysts.

关 键 词：加氢脱硫 NI-MO NA2O MCM-41 引入顺序 

分 类 号：TE624.9[石油与天然气工程—油气加工工程]