正庚烷在Ni_2P/SAPO-11催化剂上的加氢异构化反应性能
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摘要
采用次磷酸镍过量浸渍-分解法制备了Ni_2P/SAPO-11催化剂,通过低温N2吸附-脱附、XRD、HRTEM等分析手段对催化剂进行了表征。以正庚烷为原料,在固定床微反装置上考察了反应条件、Ni_2P负载量对正庚烷加氢异构化反应性能的影响,并与Pt/SAPO-11催化剂进行了对比。结果表明:Ni_2P/SAPO-11催化剂具有与Pt基催化剂相当的异构化选择性,但异构化活性和芳构化选择性较低;Ni最佳负载量(w)为4%,优化的反应条件为:反应温度400℃、压力0.5 MPa、氢烃体积比500、体积空速1h~(-1),在此条件下正庚烷的转化率为73.0%,异构化选择性为90%。
Ni_2P/SAPO-11 catalysts were prepared by decomposition of nickel hypophosphite impregnated on SAPO-11 support through excessive impregnation method and characterized by means of N_2 sorption-desorption,XRD,HRTEM techniques.The effects of reaction conditions and nickel phosphide content on hydroisomerization of n-heptane were investigated in a fixed-bed reactor and compared with Pt/SAPO-11 catalyst.The results show that Ni_2P supported on SAPO-11 molecular sieve has a high isomerization selectivity equivalent to the Pt-catalyst,however,the isomerization activity and aromatization selectivity were relatively lower.The optimum content of Ni_2P on SAPO-11 molecular sieve is 4%.At the optimal conditions:400 ℃,0.5 MPa,the volume ratio of H_2 and n-heptane of 500,and LHSV of 1h~(-1),the conversion of n-heptane and the isomerization selectivity reaches 73.0% and 90%,respectively.
Ni_2P/SAPO-11 catalysts were prepared by decomposition of nickel hypophosphite impregnated on SAPO-11 support through excessive impregnation method and characterized by means of N_2 sorption-desorption,XRD,HRTEM techniques.The effects of reaction conditions and nickel phosphide content on hydroisomerization of n-heptane were investigated in a fixed-bed reactor and compared with Pt/SAPO-11 catalyst.The results show that Ni_2P supported on SAPO-11 molecular sieve has a high isomerization selectivity equivalent to the Pt-catalyst,however,the isomerization activity and aromatization selectivity were relatively lower.The optimum content of Ni_2P on SAPO-11 molecular sieve is 4%.At the optimal conditions:400 ℃,0.5 MPa,the volume ratio of H_2 and n-heptane of 500,and LHSV of 1h~(-1),the conversion of n-heptane and the isomerization selectivity reaches 73.0% and 90%,respectively.
引文
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[3]王鲁强,郭庆洲,董维正,等.氢分压对润滑油异构降凝反应的影响[J].石油炼制与化工,2006,37(5):29-33
[4]耿承辉,高志贤,周敬来.提高非贵金属临氢脱蜡催化剂异构化能力的研究[J].燃料化学学报,2004,32(2):215-218
[5]李景峰、李学辉、柴永明,等.磷化镍的制备、表征及其催化性能研究进展[J].化工进展,2013,32(11):2621-2630
[6]李素魁,王海彦,鄢景森.磷预处理对γ-Al2O3及其负载Ni2P催化剂加氢脱硫性能影响[J].石油炼制与化工,2014,45(5):60-65
[7]鄢景森,王海彦,齐振东,等.Ni2P/TiO2-SiO2催化剂的制备、表征及其加氢脱氮反应性能评价[J].石油炼制与化工,2014,45(9):40-46
[8]Liu Lihua,Liu Shuqun.Ni2P-MoS2/γ-Al2O3catalyst for deep hydrodesulfurization via the hydrogenation reaction pathway[J].China Petroleum Processing and Petrochemical Technology,2014,16(4):12-18
[9]梁君,王福平.烷烃加氢异构化反应[J].化学进展,2008,20(4):457-463
[10]徐如人,马合元,徐翔华,等.SAPO-11构型分子筛的合成及结构研究[J].高等学校化学学报,1990,11(7):676-680
[11]Corma A,Chica A,Guil J M,et al.Determination of the pore topology of zeolite IM-5by means of catalytic test reactions and hydrocarbon adsorption measurements[J].Journal of Catalysis,2000,189(2):382-394
[12]Song Hua,Lu Mingqing.A study of catalyst for n-pentane isomerization[J].Journal of Fuel Chemistry and Technology,2003,31(3):276-279
[13]张飞,耿承辉,高志贤,等.Pt/SAPO-11临氢异构化催化剂反应特性的研究[J].燃料化学学报,2005,33(3):309-313
[14]Tian Shasha,Chen Jixiang.Hydroisomerization of n-dodecane on a new kind of bifunctional catalyst:Nickel phosphide supported on SAPO-11 molecular sieve[J].Fuel Processing Technology,2014,122(6):120-128
[15]Chao Kuei-Jung,Lin Chien-Chung,Lin Chia-Hung,et al.nHeptane hydroconversion on platinum-loaded mordenite and beta zeolites:The effect of reaction pressure[J].Applied Catalysis A:General,2000,203(2):211-220
[16]Ren Xingtao,Li Niu,Cao Jianqiu,et al.Hydroisomerization of n-decane over Pt/SAPO-41catalyst[J].Applied Catalysis A:General,2006,298(1):144-151
[17]问金盈,张树华,陈西银.正庚烷临氢异构化研究进展[J].石油大学学报(自然科学版),2001,25(6):123-128
[18]Yang Xiaomei,Ma Huaijun,Xu Zhusheng,et al.Hydroisomerization of n-dodecane over Pt/MeAPO-11(Me=Mg,Mn,Co or Zn)catalysts[J].Catalysis Communications,2007,8(8):1232-1238