La含量对Ni-S_2O_8^(2-)/ZrO_2-Al_2O_3固体超强酸催化剂结构及异构性能的影响  

Effects of La contents on the structure and isomerization performance over solid superacid Ni-S_2O_~8(2-)/ZrO_2-Al_2O_3

作　　者：宋华[1,2] 赵乐乐[1] 宋华林[3] 王娜[1] 李锋[2] 

机构地区：[1]东北石油大学化学化工学院,黑龙江大庆163318 [2]东北石油大学石油与天然气化工黑龙江省重点实验室,黑龙江大庆163318 [3]牡丹江医学院黑龙江省高校肿瘤疾病防治重点实验室,黑龙江牡丹江157011

出　　处：《中国石油大学学报（自然科学版）》2015年第5期150-156,共7页Journal of China University of Petroleum(Edition of Natural Science)

基　　金：中国石油天然气股份有限公司科技风险创新研究(07-06D-01-04-03-02)

摘　　要：制备一系列不同La质量分数的La-Ni-S2O82-/Zr O2-Al2O3催化剂(记为La-Ni-SZA),采用XRD、BET、H2-TPR、FTIR、Py-IR等手段对催化剂进行表征。以正戊烷异构化为探针反应,考察La质量分数对催化剂结构和异构化性能的影响。结果表明:引入适量的La能使催化剂中四方晶相Zr O2的颗粒尺寸减小,改善催化剂的氧化还原性能,促进L酸和B酸的形成;催化剂总酸量顺序为La(1.0)-Ni-SZA>Ni-SZA>SZA;La质量分数为1.0%的La(1.0)-Ni-SZA催化剂具有最高的异构化活性,在反应温度为140℃、压力为2.0 MPa、氢烃摩尔比为4、质量空速为1.0 h-1时,异戊烷产率达66.5%,明显高于Ni-SZA催化剂最佳反应温度(180℃)下的异戊烷产率(55.0%)。A series of La-Ni-S2O82-/ZrO2-Al2O3(La-Ni-SZA) catalysts with different La mass fractions were prepared, which were characterized by XRD, BET, H2-TPR, FTIR and Py-IR techniques. The effects of the La content on the cata-lyst structure and isomerization performance were studied using n-petane isomerization as a probe reaction. The results show that the addition of an appropriate amount of La decreases the ZrO2 particle size of tetragonal phase in the catalyst, which im-proves the redox properties of the catalyst, and promotes the formation of L acid and B acid. The total acidity of catalysts de-creases in the order of La(1. 0)-Ni-SZA>Ni-SZA>SZA. The La(1. 0)-Ni-SZA with La mass fraction of 1. 0% presents the best isomerization performance. At a reaction temperature of 140 ℃, a pressure of 2. 0 MPa, a hydrogen/hydrocarbon molar ratio of 4, and a MHSV of 1. 0 h-1 , the isopentane yield reaches a maximum of 66. 5%, which is significantly higher than the isopentane yield of Ni-SZA catalyst (55. 0%) at the optimal reaction temperature of 180 ℃.

关 键 词：镧 镍 固体超强酸 正戊烷 异构化 

分 类 号：O643.36[理学—物理化学]