Abstract: Isobutene oligomerization can be catalyzed by solid superacid SO42-/ZrO2 (SZ) at low temperature.A series of SO42-/ZrO2 (SZ) catalyst samples are prepared through direct precipitation impregnation method.The effects of liquid/solid impregnation ratio and concentration of sulfuric acid on SZ's catalytic performance are studied.The crystalline structure,acid amount and acid strength of the catalysts are characterized by XRD,NH3-TPD and TG.The results indicate that the liquid/solid impregnation ratio has a significant effect on the performance of SZ catalysts in catalyzing isobutene oligomerization.The resulting product has the highest pentamer selectivity when the liquid solid impregnation is 1.Strong acid center amount and monoclinic phase within the catalyst can be increased by lowing the concentration of sulfuric acid,which leads to great improvement of isobutene oligomerization performance of SZ catalysts.
[1] 胡云光.异丁烯聚合物的应用及合成[J].石油化工,1992,(2):125-129. [2] Ahrahamsson P,Gevert B,Jaras S.A Method of making a catalyst based on silicon dioxide and phosphoric acid:EP,0371938[P].Eur Pat Appl,1990-06-06. [3] Ji Woong Yoon,Ji Sun Lee,Sung Hwa Jhung.Oligomerization of isohutene over aluminum chloride-loadedUSY zeolite catalvsts[J].J Porous Mater,2009,16:631-634. [4] Yoon J W,Chang J S,Lee H D,et al.Trimerization of isohutene over cation exchange resins:Effect of physical properties of the resins and reaction conditions[J].Journal of Molecular Catalysis A:Chemical,2006,260:181-186. [5] Bellussi G,Brunelli M,Castelvetro W,et al.Catalyst and process for oligomerizing olefins:US,5510555[P].1994-02-10. [6] 段红玲,刘雪暖,罗祥生.异丁烯齐聚催化剂硫酸铁-硫酸镍的性能评价[J].青岛科技大学学报自然科学版,2009,30(4):317-320. [7] 候祥麟.中国炼油技术[M].北京:中国石化出版社,2001:234. [8] 金照生,徐菁,袁梅卿,等.用于异丁烯选择性二聚的催化剂:CN 2005100236161[P].2005-01-26. [9] 温陵生,刘雅娟,张武阳,等.固体磷酸催化剂的活性相[J].高等学校化学学报,1994,15(3):428-430. [10] 杨淑清,郑贤敏,王路辉,张仁坤,王东光.三氯化铁离子液体催化异丁烯的齐聚反应[J].化工学报,2016,67(S1):276-282. [11] 马克存,徐婷婷,马立莉.异丁烯齐聚催化剂的研究进展[J].炼油与化工,2017,28(4):1-4. [12] Hino M,Kobayashi S,Arata K.Reactions of butane and isobutene catalyzed by zirconium oxide treated with sulfate Ion.Solid superacid catalyst[J].Journal of the American Chemical Society,1979,101:6439-6441. [13] Hong Z,Fogash K B,Dumesic J A.Reaction kinetic behavior of sulfated-zirconia catalysts for butane isomerization[J].Catalysis Today,1999,51:269-288. [14] Song X,Sayari A.Sulfated zirconia-based strong solid-acid catalysts recent progress[J].Catalysis Reviews:Science and Engineering,1996,38:329-412. [15] Yamaguchi T.Application of ZrO2 as a catalyst and a catalyst support[J].Catalysis Today,1994,20;199-208. [16] Yoon J W,Jhung;S H,Kim T J,et al.Trimerizatiun of isobutene over solid acid catalysts under wide reaction conditions[J].Bulletin-Korean Chemical Society,2007,28(11):2075-2078. [17] Ji Sun Lee,Ji Woong Yoon,Shiva B Halligudi,et al.Trimerization of isobutene over WO<em>x/ZrO2 catalysts[J].Applied Catalysis A:General,2009,366(2):299-303. [18] de Klerk,A.Oligomerization of 1-hexene and 1-octene over solid acid catalysts[J].Industrial & Engineering Chemistry Research,2005,44(11):3887-3893. [19] Ji Woong Yoon,Sung Hwa Jhung,Dae Hyun Choo,et al.Oligomerization of isobutene over dealuminated Y zeolite catalysts[J].Applied Catalysis A:General,2008,337:73-77. [20] 乐晓光,徐俊,宋月芹,等.制备条件对Pt/SO42-/ZrO2-Al2O3异构化性能的影响[J].化工进展,2015,34(2):419-424. [21] Yang Y C,Weng H S.Al-promoted Pt/SO42-/ZrO2 with low sulfate content for n-heptane isomerization[J].Applied Catalysis A:General,2010,384:94-100. [22] Yadav G D,Murkute A D.Preparation of the novel mesoporous solid acid catalyst UDCaT-4 via synergism of persulfated alumina and zirconia into hexagonal mesoporous silica for allcylation reactions[J].Advanced Synthesis & Cattalysis,2004,346:389-394. [23] Benitez V M,Yori J C,Vera C R,et al.Characterization of transition-metal oxides promoted with oxoanions by means of test reactions[J].Industrial & Engineering Chemistry Research,2005,44:1716-1721. [24] Sun Y,Walspurger S,Louis B,et al.Investigation of factors influencing activityfor n-butane isomerization in the presence of hydrogen on Al-promoted sulfated zirconia[J].Applied Catalysis A:General,2005,292:200-207. [25] 申延明,戎梅竹,刘宏伟,等.SO42-/ZrO2固体超强酸的制备及其催化合成ETBE的研究[J].石油炼制与化工,2006,37(8):12-15.
