陈化温度对导向剂法制备SAPO-11分子筛及异构化性能的影响
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摘要
采用导向剂法在不同陈化温度下成功合成SAPO-11分子筛。利用XRD、N_2吸附-脱附等温曲线,BET物理吸附,NH3-TPD以及扫描电镜(SEM)等方法对分子筛的形貌,酸性质以及孔结构性质进行分析表征。以正十二烷为原料,考察Pt负载量为0. 5%的Pt/SAPO-11催化剂的异构化反应催化性能。结果表明:不同陈化温度影响催化剂的性能,陈化温度为120℃合成的SAPO-11分子筛具有最优性能,晶粒尺寸约为2μm,BET总比表面积为208. 8 m~2·g~(-1),正十二烷加氢异构化的异构烃收率最高达66. 7%。
SAPO-11 molecular sieves were successfully synthesized by the guidance agent method at different aging temperatures. The morphology,acid properties and pore structure of molecular sieve were characterized by physical adsorption of NH_3-TPD and scanning electron microscope( SEM). The hydroisomerization performance of Pt/SAPO-11 catalyst loaded with 0. 5% chloroplatinic acid was investigated by using n-dodecane of long-chain alkanes as raw material. The results show that different aging temperatures affect the performance of the catalyst. When the aging temperature is 120 ℃,the SAPO-11 molecular sieve has the best performance,the grain size is about 2 μm BET total specific surface area is up to 208. 8 m~2·g~(-1),and the iso-hydrocarbon yield of dodecane hydroisomerization is up to 66. 7%.
SAPO-11 molecular sieves were successfully synthesized by the guidance agent method at different aging temperatures. The morphology,acid properties and pore structure of molecular sieve were characterized by physical adsorption of NH_3-TPD and scanning electron microscope( SEM). The hydroisomerization performance of Pt/SAPO-11 catalyst loaded with 0. 5% chloroplatinic acid was investigated by using n-dodecane of long-chain alkanes as raw material. The results show that different aging temperatures affect the performance of the catalyst. When the aging temperature is 120 ℃,the SAPO-11 molecular sieve has the best performance,the grain size is about 2 μm BET total specific surface area is up to 208. 8 m~2·g~(-1),and the iso-hydrocarbon yield of dodecane hydroisomerization is up to 66. 7%.
引文
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[15]Zhang F,Liu Y,Sun Q,et al.Design and Preparation of Efficient Hydroisomerization Catalysts by The Formation of Stable SAPO-11 Molecular Sieve Nanosheets with 10-20 nm Thickness and Partially Blocked Acidic Sites[J].Chemical Communications.2017,53(36):42-49.
[16]吴海琳,王海彦,吴晓娜,等.间接模板剂法合成介孔SAPO-11分子筛及其加氢异构化性能[J].硅酸盐学报,2018,46(10):1-6.
[17]王利军,黄茜丹,赵伟,等.SAPO-11分子筛改进合成及正十二烷加氢异构化性能[J].化学学报,2002,60(6):1122-1124.
[18]柳云骐,田志坚,徐竹生,等.正构烷烃在双功能催化剂上异构化反应研究进展[J].中国石油大学学报:2002,26(1):123-129.
[2]罗小林,陈亚芍,常鹏梅,等.离子胶束诱导微波合成SAPO-11分子筛微球[J].物理化学学报,2009,25(1):137-144.
[3]韩磊.超细SAPO-11分子筛制备及其异构化性能[D].青岛:中国石油大学(华东),2013.
[4]肖寒,于海斌,刘红光,等.晶种硅烷化合成小粒径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.
[5]Guo L,Bao X J,Fan Y,et al.Impact of Cationic Surfactant Chain Length During SAPO-11 Molecular Sieve Synthesis on Structure,Acidity,and n-octane Isomerization to Dimethyl Hexanes[J].Journal of Catalysis,2012,294(10):161-170.
[6]徐铁钢,吴显军,王刚,等.轻质烷烃异构化催化剂研究进展[J].化工进展,2015,34(2):397-401.
[7]谢敏慧,齐学振,刘学军,等.SAPO-11的制备及正十八烷异构性能研究[J].分子催化,2016,30(6):515-522.
[8]于中伟,孙义兰,任坚强,等.固体超强酸催化C5/C6烷烃异构化反应[J].石油学报(石油加工),2010,26(1):88-92.
[9]Doadrio A L,Sousa E M,Pariente J P,et al.Mesoporous SBA-15 HPLC Evaluation for Controlled Gentamicin Drug Delivery[J].Journal of Controlled Release,2004,97(1):125-132.
[10]任建生.轻质烷烃异构化工艺技术[J].炼油技术与工程,2013,43(7):28-31.
[11]Yang X,Lu T,Chen C,et al.Synthesis of Hierarchical AIPO-n Molecular Sieves Templated by Saccharides[J].Micropor Mesopor Mater,2011,144(1):176-182.
[12]杨娜,岳明波,王一萌,等.干胶法合成分子筛[J].化学进展,2012(2):253-261.
[13]苏彤.SAPO-11分子筛的合成及其烷烃异构反应研究[D].西安:西安石油大学,2015.
[14]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.
[15]Zhang F,Liu Y,Sun Q,et al.Design and Preparation of Efficient Hydroisomerization Catalysts by The Formation of Stable SAPO-11 Molecular Sieve Nanosheets with 10-20 nm Thickness and Partially Blocked Acidic Sites[J].Chemical Communications.2017,53(36):42-49.
[16]吴海琳,王海彦,吴晓娜,等.间接模板剂法合成介孔SAPO-11分子筛及其加氢异构化性能[J].硅酸盐学报,2018,46(10):1-6.
[17]王利军,黄茜丹,赵伟,等.SAPO-11分子筛改进合成及正十二烷加氢异构化性能[J].化学学报,2002,60(6):1122-1124.
[18]柳云骐,田志坚,徐竹生,等.正构烷烃在双功能催化剂上异构化反应研究进展[J].中国石油大学学报:2002,26(1):123-129.