非负载NiMoS和NiWS催化剂组成对其结构、形貌和加氢脱氮性能的影响  

Effect of composition on structure,morphology and hydrodenitrogenation performance over unsupported NiMoS and NiWS catalysts

作　　者：刘欣毅[1,2] 刘铁峰 蒋宗轩[1] 李灿[1] Liu Xinyi;Liu Tiefeng;Jiang Zongxuan;Li Can(State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian Liaoning 116023,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023 [2]中国科学院大学,北京100049

出　　处：《石油化工》2021年第10期1004-1012,共9页Petrochemical Technology

基　　金：中国科学院科技服务网络计划项目(KFJ-STS-QYZX-015)。

摘　　要：以含Ni层状双氢氧化合物(Ni-LDH)为结构模板制备了一系列非负载双金属NiMoS和NiWS催化剂。以喹啉为模型含氮化合物评价了催化剂的加氢脱氮(HDN)性能,并通过XRD、N_(2)吸附-脱附、SEM、TPS等手段分别对催化剂进行了表征。表征结果显示,Mo/W组分的引入能够显著降低催化剂的颗粒尺寸,有利于形成更多活性中心;但过量Mo/W组分的存在也会导致催化剂颗粒的聚集,反而不利于活性位点的暴露。实验结果表明,当Mo(W)/Ni摩尔比为0.3时催化剂表现出最高的HDN活性;此外,当Mo(W)/Ni摩尔比超过0.3时,由于对颗粒的分散作用有限,MoS2/WS2晶粒的堆积层数有所增加,使得氢解活性位点数目的比例增大,氢解选择性升高。A series of layered unsupported bimetallic NiMoS and NiWS catalysts were prepared by using Ni layered double hydroxides(Ni-LDH)as a structural template.The catalytic performance was evaluated for quinoline hydrodenitrogenation(HDN)performance of catalyst was evaluated by quinoline.The catalysts were characterized by XRD,N_(2) adsorption-desorption,SEM and TPS.The characterization results show that the introduction of Mo/W significantly reduce the catalyst particle size,which is conducive to the formation of the catalytic active sites.However,the excessive Mo/W components also lead to an aggregation of the catalyst particles,which is detrimental to the exposure of active sites on the particle surface.The evaluation results show that the catalysts with a Mo(W)/Ni molar ratio of 0.3 exhibit the highest HDN activity.In addition,when the Mo(W)/Ni molar ratio is larger than 0.3,owing to the limited dispersive effect on the catalyst particles,the stacking numbers of MoS2/WS2 crystallites also increase with increasing the Mo(W)/Ni molar ratio,resulting in an increase in the ratio of the hydrolysis active sites and the hydrolysis selectivity.

关 键 词：非负载催化剂 加氢脱氮 层状双氢氧化合物 

分 类 号：TQ032.41[化学工程]