醇-水体系SAPO-11分子筛的合成及其异构化性能
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摘要
分别以甲醇、乙醇、异丙醇替代部分或全部的水,采用静态法水热合成SAPO-11分子筛,考察了醇的种类以及醇的替代量对产物晶型结构、形貌、酸性以及催化性能的影响。以正十二烷为原料,考察Pt质量分数为0. 5%的SAPO-11分子筛的异构化反应性能。结果表明,利用乙醇完全替代水为溶剂合成的SAPO-11分子筛具有较大的BET比表面积和更温和的酸性,在正十二烷的临氢异构化反应中表现出优异的催化性能。在反应温度为340℃、反应空速为1. 0 h~(-1)、反应压力为2 MPa、氢与油体积比为200∶1条件下,正十二烷转化率为91. 65%,异构烃收率为66. 27%。
SAPO-11 molecular sieve is synthesized via static hydrothermal method with methanol,ethanol and isopropanol respectively instead of some or all water.The effects of alcohol types and alcohol substitution amount on the crystal structure,morphology,acidity and catalytic performance of SAPO-11 molecular sieve are investigated.The catalytic properties of SAPO-11 molecular sieve with 0. 5% Pt loading( mass fraction) in isomerization are investigated by using n-dodecane as raw material.The results show that SAPO-11 molecular sieve synthesized with ethanol instead of water has larger BET specific surface area and milder acidity,and has excellent catalytic performance in hydroisomerization of ndodecane.Over the SAPO-11 molecular sieve synthesized with ethanol instead of water,the conversion of n-dodecane can reach 91. 65% and the yield of iso-hydrocarbon can reach 66. 27% when the reaction temperature is set at 340℃,the reaction space velocity is 1. 0 h~(-1),the reaction pressure is 2 MPa and the ratio of hydrogen to oil volume is 200 ∶1.
SAPO-11 molecular sieve is synthesized via static hydrothermal method with methanol,ethanol and isopropanol respectively instead of some or all water.The effects of alcohol types and alcohol substitution amount on the crystal structure,morphology,acidity and catalytic performance of SAPO-11 molecular sieve are investigated.The catalytic properties of SAPO-11 molecular sieve with 0. 5% Pt loading( mass fraction) in isomerization are investigated by using n-dodecane as raw material.The results show that SAPO-11 molecular sieve synthesized with ethanol instead of water has larger BET specific surface area and milder acidity,and has excellent catalytic performance in hydroisomerization of ndodecane.Over the SAPO-11 molecular sieve synthesized with ethanol instead of water,the conversion of n-dodecane can reach 91. 65% and the yield of iso-hydrocarbon can reach 66. 27% when the reaction temperature is set at 340℃,the reaction space velocity is 1. 0 h~(-1),the reaction pressure is 2 MPa and the ratio of hydrogen to oil volume is 200 ∶1.
引文
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[14]刘国柱,韩立军,师亚威.Pt/SAPO-11催化费托合成油选择性加氢异构化制备替代喷气燃料[J].石油化工,2015,44(2):144-149.
[2]Brent M,Messina A,Edith M.Silicoaluminophosphate molecular sieves:Another new class of microporous crystalline inorganic solids[J].J Am Chem Soc,1984,106(20):6092-6093.
[3]田辉平,袁健兵,朱泽霖,等.SAPO-11分子筛用i-Pr2NH导向合成及其酸性性质[J].燃料化学学报,1997,25(6):514-518.
[4]汪哲明,阎子峰.丁烯骨架异构化催化剂进展[J].石油化工,2002,31(4):514-518.
[5]汪哲明,阎子峰.新型取代型磷酸铝分子筛的合成与表征[J].燃料化学学报,2001,29:9-11.
[6]Sugmoto M,Katsuno H,Takasu K,et al.Correlation between the crystal zize and catalytic properties of ZSM-5 zeolites[J].Zeolites,1987,7(6):503-507.
[7]Jindrich H,Hansidaar S,Nienhuis J Q,et al.The role of deposits in butene isomerisation[J].J Catal,1999,176(1):83-89.
[8]张胜振,陈胜利,董鹏,等.小晶粒SAPO-11分子筛的合成及其催化异构化性能[J].催化学报,2007,28(10):857-864.
[9]肖寒,于海斌,刘红光,等.晶种硅烷化合成小晶粒SAPO-11分子筛表征及其临氢异构化催化性能评价[J].石油炼制与化工,2014,45(1);28-34.
[10]Viaplana-marin I,Fernandez-borras J,Blasco J.Effects of the protein/carbohydrate ratio of extruded diets on protein synthesis,protein growth and body composition in juvenile brown trout(Salmo trutta)[J].Aquaculture International,2006,242(1):153.
[11]Kalita B,Talukdar A K.An effcient synthesis of nanocrystalline MFIzeolite using different silica sources:A green approach[J].Mate Res Bull,2009,44(2):254-258.
[12]Mintova S,Valtchev V.Effect of the silica source on the formation of nanosized silicalite-1:An in situ dynamic light scattering study[J].Microporous Mesoporous Mater,2002,55(2):171-179.
[13]Gregg S J,Sing K S W.Adsirption,surface area and porosity[M].London:Academic Press,1982:154.
[14]刘国柱,韩立军,师亚威.Pt/SAPO-11催化费托合成油选择性加氢异构化制备替代喷气燃料[J].石油化工,2015,44(2):144-149.