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采用水热合成法,将未焙烧的介孔材料SBA-15作为硅源合成介孔SAPO-11分子筛。利用X射线衍射、N2吸附-脱附等温曲线,BET物理吸附,NH3-TPD以及扫描电子显微镜等对分子筛的形貌和孔结构性质进行表征。将正十二烷作为原料,考察负载量为0.5%的Pt/SAPO-11分子筛催化剂的加氢异构化反应催化性能。结果表明:以未焙烧的SBA-15作为硅源制备介孔SAPO-11分子筛,介孔比表面积为77.2 m2/g以及介孔孔容为0.261 m3/g,有效降低孔道传质阻力,酸量显著增加,活性位增多,使长链烷烃加氢异构化的选择性达到65.21%。
Abstract:The hierarchical SAPO-11 molecular sieves were synthesized by a hydrothermal method with mesoporous material SBA-15 as a silica source. The morphology and the pore structure of zeolites were characterized by X-ray diffraction and N2 adsorption-desorption isothermal analysis, specific surface area measurement, NH3-TPD and scanning electron microscopy respectively. The catalyst loading of hydroisomerization catalytic performance of Pt/SAPO-11 molecular sieve prepared with dodecane is 0.5%. The result shows that the uncalcined SBA-15 can be used as a silica source for the synthesis of mesoporous SAPO-11 molecular sieve with the mesoporous specific surface area of 77.2 m2/g and the mesoporous volume of 0.261 m3/g. This sieve can effectively reduce the pore mass transfer resistance, and increase the number of active sites, and the selectivity of long chain alkanes hydroisomerization reaches 65.21%.
[1]LOKBM,MESSINACA,PATTONRL,etal.Silicoalum inophosphatemolecularsieve:Anothernewclassofmicroporous crystallineinorganicsolids[J].JAmChemSoc,1984,106(20):6092–6093.
[2]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.ZHANG Shengzhen, CHEN Shengli, DONG Peng, et al. Chin J Catal(in Chinese), 2007, 28(10):857-864.
[3]汪哲明,阎子峰.新型ZrAPO-11分子筛的合成与表征[J].燃料化学学报, 2001, 29(1):9–11.WANGZheming,YANZifeng.JFuelChemTechnol(inChinese),2001, 29(1):9-11.
[4]李晓辉. SAPO-11分子筛催化剂在正庚烷异构化性能的研究[D].大庆:大庆石油学院, 2010.LIXiaohui,Studyonisomerizationofn-heptaneoverSAPO-11molecularsievecatalyst(inChinese,dissertation)Daqing:Daqing Petroleum Institute, 2010.
[5]SINHA A K, SEELAN S. Characterization of SAPO-11 and SAPO-31synthesizedfromaqueousandnonaqueousmedia[J].ApplCatalB,2004, 270(1/2):245–252.
[6]YANGX,LUT,CHENC,etal.SynthesisofhierarchicalAIPO-n molecularsievestemplatedbysaccharides[J].MicroporMesopor Mater, 2011, 144(1/3):176-182.
[7]胡健,王建伟,田松柏.SAPO分子筛在烃类异构化反应中的应用[J].化工进展, 2005, 24(11):121–122.HUJian,WANGJianwei,TIANSongbai.JProgressChemInd(in Chinese), 2005, 24(11):121–122.
[8]宋磊,介孔材料简介及其制备方法[J].新疆有色金属,2011,34(1):122–124.SONGLei,JXinjiangNonferrousMet(inChinese),2011,34(1):122–124.
[9]LOPEZS,INAYATA,SCHWABA,etal.Zeoliticmaterialswith hierarchical porous structures[J]. Adv Mater, 2011, 23(22/23):2602–2615.
[10]DOADRIO,AL,SOUSA,EMB,Doadrio,JC,etal.Mesoporous SBA-15 HPLC evaluation for controlled gentamicin drug delivery[J]. J Controlled. Release, 2004, 97(1):125–132.
[11]ZHUYF,SHIJL,WANGSH,etal.Stimuli-responsivecontrolled drugreleasefromahollowmesoporoussilicasphere/polyelectrolyte multilayer coreshell structure[J]. Angew Chem Int Edit, 2010, 117(32):5213–5217.
[12]孙娜,王海彦,李浩.剑麻纤维素合成多级孔SAPO-11分子筛及其临氢异构化性能[J].硅酸盐学报, 2018, 46(1):109–114.SUNNa,WANGHaiyan,LIHao.JChinCeramSoc,2018,46(1):109–114.
[13]刘振,马志鹏,孙常庚.硬模板法制备微孔-介孔复合SAPO-11分子筛及其长链烷烃异构化反应[J].中国石油大学学报:自然科学版,2014, 38(2):153–158.LIU Zhen, MA Zhipeng, SUN Changgeng. China Unive Petr:Nat Sci(in Chinese), 2014, 38(2):153–158.
[14]刘远林.多孔磷酸硅铝分子筛SAPO-34的合成及其在MTO反应中的应用[D].上海:华东理工大学, 2010.LIUYuanlin,Synthesisofporousaluminumsilicatephosphate molecularsieveSAPO-34anditsapplicationinMTOreaction(in Chinese, dissertation). Shanghai:East China University of Science and Technology, 2010.
[15]汪哲明,阎子峰,SAPO-11分子筛的合成[J].燃料化学学报,2003,31(4):360–366.WANGZheming,YANZifeng.JFuelChemTechnol(inChinese),2003, 31(4):360-366.
[16]WUQ,ODUROIN,HUANGY,etal.SynthesisofHierarchical SAPO-11viaSeededCrystallization[J].MicroporMesoporMater,2015, 218:24–32.
[17]YANGSM,LINJY,GUODH,etal.1-Buteneisomerizationover aluminophosphatemolecularsievesandzeolites[J].ApplCatalA:General, 1999, 181(1):113–122.
[18]WALENDZIEWSKIJ,PNIAKB.Synthesis,physicochemical propertiesandhydroisomerizationactivityofSAPO-11based catalysts[J]. Appl Catal A:General, 2003, 250(1):39–47.
[19]SARAH C L. Nanocrystalline zeolites and zeolite strutures:Synthesis,characterizationandapplication[J].JPhysChemC,2007,111(50):18464-18474.
[20]CLAUDEMC,MARTENSJA.Monomethylbranchingoflong n-alkaneintherangefromdecanetotetracosaneonPt/HZSM-22Bi-function catalyst[J]. J Catal, 2000, 190(1):39-48.
基本信息:
DOI:10.14062/j.issn.0454-5648.2018.10.15
中图分类号:O643.36
引用信息:
[1]吴海琳,孙娜,王海彦,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):1447-1452.DOI:10.14062/j.issn.0454-5648.2018.10.15.
基金信息:
国家自然科学基金项目(2016-Z0030)
2018-07-26
2018-07-26
2018-07-26