nMoO_x·USY加氢脱硫性能的研究  

An investigation on the hydrodesulrization performance of nMoO_x·USY

作　　者：苗杰 李双 迟姚玲 李明航 谈冠希 靳广洲 Miao Jie;Li Shuang;Chi Yaoling;Li Minghang;Tan Guanxi;Jin Guangzhou(School of Chemical Engineering,Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology,Beijing Institute of Petrochemical Technology,Beijing 102617,China;Department of Biology,Bejing University of Chemical Technology,Beijing 100029,China)

机构地区：[1]北京石油化工学院化学工程学院燃料清洁化及高效催化减排技术北京市重点实验室,北京102617 [2]北京化工大学化学工程学院,北京100029

出　　处：《石油化工》2019年第9期892-898,共7页Petrochemical Technology

基　　金：国家重点基础研究发展计划项目（2012CB215002）

摘　　要：以柠檬酸络合法和等体积浸渍法制备了不同Mo含量的nMoOx·USY单相复合体催化剂,并在自制的高压微反装置上,以二苯并噻吩/正癸烷溶液为模型反应物评价了nMoOx·USY单相复合体催化剂的加氢脱硫活性。采用XRD,BET,SEM,NH3-TPD等方法对催化剂试样的物相结构、表面形貌、比表面积、孔体积、平均孔径、表面酸性等进行了表征。表征结果显示,Mo物种借助固相反应以MoOx簇的形式进入并定位于USY分子筛体相笼中形成nMoOx·USY单相复合体,引起USY分子筛晶胞收缩,晶胞参数减小,比表面积下降,弱酸中心占比增多,强酸中心占比减少,总酸量增多。实验结果表明,在反应压力4.0 MPa、液态空速20 h-1、氢油体积比600∶1的条件下,试样nMoOx·USY-8的加氢脱硫转化率最高,分别达到71.78%,96.18%,99.39%;nMoOx·USY催化剂的二苯并噻吩脱硫反应主要以加氢脱硫途径进行。The nMoOx·USY single-phase complex catalysts with different content of Mo was prepared by citric acid complex and incipient impregnation methods.The hydrodesulfulrization performance of the nMoOx·USY was evaluated by using dibenzothiophene/n-decane as model reactant in a self-made high-pressure-micro-reactor,and the phase structure,surface topography,specific surface area,pore volume,average pore width and surface acidity of the catalyst sample were characterized by XRD,BET,SEM and NH3-TPD methods.The characterization results indicated that the nMoOx·USY single-phase complex was prepared by using solid-state reaction of Mo speciation to enter and locate in USY molecular sieve cage in the form of MoOx clusters.It induced the contraction of the molecular sieve lattice cell,the decrease of the lattice parameters and specific surface area.The total acid amount and the proportion of the weak acid sites was increased,the proportion of the strong acid sites was decreased.The experimental results show that sample nMoOx·USY-8 had the highest hydrodesulfurization conversion rate which reached 71.78%,96.18%,99.39%under the reaction conditions of 4.0 MPa,LHSV 20 h-1 and H2/oil volume ratio 600∶1.The dibenzothiopene desulfurization reaction of the nMoOx·USY catalyst was dominated by the hydrogenation route.

关 键 词：nMoOx·USY单相复合体 二苯并噻吩 加氢脱硫 转化率 

分 类 号：TQ426.61[化学工程]