微波水热法制备含磷W/Al_2O_3催化剂及其加氢脱氮性能  

Preparation of phosphorous-containing W/Al_2O_3 catalysts via microwave hydrothermal method and their hydrodenitrogen activity

作　　者：王豪[1] 赵婉莹[1] 刘振伟[1,2] 尧振宇 吴雁[1] 

机构地区：[1]西南石油大学化学化工学院,四川成都610500 [2]中国石油独山子石化公司炼油厂,新疆克拉玛依833699

出　　处：《化工进展》2015年第6期1646-1651,共6页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金项目(20906075)

摘　　要：采用微波水热法(MWH)制备含磷W/Al2O3加氢精制催化剂,分别以磷酸(PA)、磷酸三乙酯(TEP)和羟基乙叉二磷酸(HEDP)为磷源,考察磷源、制备方法和磷含量对催化剂物化性质和加氢脱氮(HDN)性能的影响。结果表明,使用HEDP为磷源不仅可减弱活性组分-载体间的相互作用,其结构中的羟基还可与MWH产生的H2WO4形成氢键而吸附在H2WO4表面,抑制H2WO4团聚,从而实现WO3的高分散。MWH快速均匀加热的特点可以有效抑制H2WO4的过度生长,并促进其在Al2O3表面的均匀快速分散,使得以HEDP为磷源制备的W/Al2O3中WO3的分散度和HDN活性远高于浸渍法制备的相同磷源、磷含量和金属含量的催化剂。MWH法制备的磷质量分数为3%的催化剂兼具高的WO3分散度和弱的WO3-Al2O3相互作用,有最佳的HDN活性。Phosphorous-containing W/Al2O3 hydrotreating catalysts were prepared via microwave hydrothermal （MWH） method,in which phosphoric acid （PA）,triethyl phosphate （TEP） and 1-hydroxy ethylidene-1,1-diphosphonic acid （HEDP） were used as phosphorus sources,respectively. The effects of phosphorus sources,catalyst preparation methods and phosphorus contents on the physicochemical properties and hydrodenitrogenation （HDN） activity of catalysts were studied. The results show that the introduction of HEDP can weaken tungsten-alumina interaction and keep highly dispersed tungsten species by forming H-bonding between the hydroxyl groups of HEDP and H2WO4 to prevent tungsten species from aggregation. The MWH method,characterized by rapid and uniform heating,can greatly inhibit the excess growth of H2WO4 colloids and help to disperse tungsten oxide on alumina uniformly and quickly. When the HEDP is used as phosphorus resource,catalyst prepared via MWH method shows much higher WO3 dispersion and HDN activity than that with the same phosphorus and metal contents prepared by impregnation method. The catalyst prepared via MWH method with 3%phosphorus combines high WO3 dispersion with weak tungsten-alumina interaction,leading to the highest HDN activity.

关 键 词：催化剂 加氢 微波 水热 磷 

分 类 号：TQ426[化学工程]