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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

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【作者】 刘欣毅刘铁峰蒋宗轩李灿

【Author】 Liu Xinyi;Liu Tiefeng;Jiang Zongxuan;Li Can;State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences;University of Chinese Academy of Sciences;

【通讯作者】 李灿;

【机构】 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中国科学院大学

【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、N2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。

【Abstract】 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,N2 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.

【基金】 中国科学院科技服务网络计划项目(KFJ-STS-QYZX-015)
  • 【文献出处】 石油化工 ,Petrochemical Technology , 编辑部邮箱 ,2021年10期
  • 【分类号】TE624.55
  • 【下载频次】178
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