蒸汽辅助合成STW结构硅锗酸盐分子筛
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摘要
采用蒸汽辅助法制备了高稳定性STW结构硅锗酸盐分子筛.相比于传统水热方法,使用温和的蒸汽辅助可显著减少模板剂用量,产物结晶度与骨架Si元素含量更高.利用X射线衍射(XRD)、扫描电子显微镜(SEM)、能量散射谱(EDS)、热重(TG)分析等技术手段考察了蒸汽辅助合成硅锗酸盐分子筛过程中水对产物结构的影响,发现随着外加水量的增加,产物从纯相Ge O2逐渐转化为STW分子筛纯相,最终变为Ge O2,STW与MFI结构的混相;此外,反应物中带入的痕量水可以优先活化Ge元素,从而在一定程度上决定了产物构型.
STW-zeotype germanosilicate was synthesized via the steam-assisted conversion(SAC) approach with N,N'-diethylethylenediamine(DEEDA) as an organic template. The effect of additional water on the resultant materials was systematically investigated by powder X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive spectrometer(EDS) and thermogravimetric(TG) analyses. In comparison with the conventional hydrothermal synthesis,the SAC method needs significantly less organic templates,through which the synthesized germanosilicate exhibits a high crystallinity and much more Si element content,as well as the high structural stability. The framework of STW-zeotype germanosilicate prepared by the SAC method remains stable even after undergoing a high temperature calcination(600 ℃).
STW-zeotype germanosilicate was synthesized via the steam-assisted conversion(SAC) approach with N,N'-diethylethylenediamine(DEEDA) as an organic template. The effect of additional water on the resultant materials was systematically investigated by powder X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive spectrometer(EDS) and thermogravimetric(TG) analyses. In comparison with the conventional hydrothermal synthesis,the SAC method needs significantly less organic templates,through which the synthesized germanosilicate exhibits a high crystallinity and much more Si element content,as well as the high structural stability. The framework of STW-zeotype germanosilicate prepared by the SAC method remains stable even after undergoing a high temperature calcination(600 ℃).
引文
[1] Zhang R.,Liu N.,Lei Z.,Chen B.,Chem. Rev.,2016,116(6),3658—3721
[2] Perego C.,Bosetti A.,Ricci M.,Millini R.,Energy Fuels,2017,31(8),7721—7733
[3] Davis M. E.,Chem. Mater.,2014,26(1),239—245
[4] Dapsens P. Y.,Mondelli C.,Pérez-Ramírez J.,Chem. Soc. Rev.,2015,44(20),7025—7043
[5] Dusselier M.,Davis M. E.,Chem. Rev.,2018,118(11),5265—5329
[6] Zimmermann N. E. R.,Haranczyk M.,Crystal Growth Design,2016,16(6),3043—3048
[7] Cheng J.,Xu R.,Yang G.,J. Chem. Soc.,Dalton Trans.,1991,92(6),1537—1540
[8] Corma A.,Navarro M. T.,Rey F.,Rius J.,Navarro S. V.,Rey M. T.,Rius F.,Valencia J. S.,Angew. Chem. Int. Ed.,2001,40(12),2277—2280
[9] Corma A.,Navarro M. T.,Rey F.,Valencia S.,Chem. Commun.,2001,(18),1720—1721
[10] Kots P. A.,Sushkevich V. L.,Tyabikov O. A.,Ivanova I. I.,Micro. Meso. Mater.,2017,243,186—192
[11] Liu X.,Chu Y.,Wang Q.,Wang W.,Wang C.,Xu J.,Deng F.,Solid State Nuclear Magnetic Resonance,2017,87,1—9
[12] Liu D. R.,Gao Z. H.,Zi W. W.,Zhang J.,Du H. B.,Chen F. J.,Micro. Meso. Mater.,2019,276,232—238
[13] Liu X.,Xu H.,Zhang L.,Han L.,Jiang J.,Oleynikov P.,Chen L.,Wu P.,ACS Catal.,2016,6(12),8420—8431
[14] Bai R.,Sun Q.,Wang N.,Zou Y.,Guo G.,Iborra S.,Corma A.,Yu J.,Chem. Mater.,2016,28(18),6455—6458
[15] Tang L.,Shi L.,Bonneau C.,Sun J.,Yue H.,Ojuva A.,Lee B. L.,Kritikos M.,Bell R. G.,Bacsik Z.,Nat. Mater.,2008,7(5),381—385
[16] Rojas A.,Arteaga O.,Kahr B.,Camblor M. A.,J. Am. Chem. Soc.,2013,135(32),11975—11984
[17] Zhang N.,Shi L.,Yu T.,Li T.,Hua W.,Lin C.,J. Solid State Chem.,2015,225,271—277
[18] Shi L.,Yu T. T.,Lin S.,Yuan Y. B.,Wang J. K.,Zhang N.,Chem. J. Chinese Universities,2015,36(8),1467—1471(石磊,于婷婷,林森,袁玉斌,王济凯,张娜.高等学校化学学报,2015,36(8),1467—1471)
[19] Moeller K.,Yilmaz B.,Jacubinas R. M.,Mueller U.,Bein T.,J. Am. Chem. Soc.,2011,133(14),5284—5295
[20] Kubu M.,Millini R.,ilkováN.,Catal. Today,2019,324,3—14
[21] Jabri H. A.,Miyake K.,Ono K.,Nakai M.,Hirota Y.,Uchida Y.,Miyamoto M.,Nishiyama N.,Micro. Meso. Mater.,2019,278,322—326
[22] Zheng J.,Lin D.,Liu Z.,Zhu K.,Zhou X.,Yuan W.,Ind. Eng. Chem. Res.,2018,57(2),548—558
[23] Rimaz S.,Halladj R.,Askari S.,J. Colloid Inter. Sci.,2016,464,137—146
[24] Zhou D.,Lu X.,Xu J.,Yu A.,Li J.,Deng F.,Xia Q.,Chem. Mater.,2012,24(21),4160—4165
[25] Neumann G. T.,Hicks J. C.,Cryst. Growth Des.,2013,13(4)1535—1542
[26] Chen Y.,Li C.,Wang L.,Zhang M.,Liang C.,Micro. Meso. Mater.,2017,252,146—153
[27] Velaga B.,Peela N. R.,Micro. Meso. Mater.,2019,279,211—219
[28] Shi L.,Wang J.,Li N.,Lin S.,J. Alloys Compounds,2017,695,2488—2498
[29] Shi L.,Wang J.,Lin S.,Sun J.,Mater. Lett.,2017,186,382—385
[30] Cheng X.,Mao J.,Lv X.,Hua T.,Cheng X.,Long Y.,Tang Y.,J. Mater. Chem. A,2014,2(5),1247—1251
[31] Zhang L.,Huang Y.,J. Phys. Chem. C,2016,120(45),25945—25957
[32] Du Q.,Guo Y.,Wu P.,Liu H.,Micro. Meso. Mater.,2018,264,272—280
[33] Rao P. R. H. P.,Matsukata M.,Chem. Commun.,1996,(12),1441—1442
[2] Perego C.,Bosetti A.,Ricci M.,Millini R.,Energy Fuels,2017,31(8),7721—7733
[3] Davis M. E.,Chem. Mater.,2014,26(1),239—245
[4] Dapsens P. Y.,Mondelli C.,Pérez-Ramírez J.,Chem. Soc. Rev.,2015,44(20),7025—7043
[5] Dusselier M.,Davis M. E.,Chem. Rev.,2018,118(11),5265—5329
[6] Zimmermann N. E. R.,Haranczyk M.,Crystal Growth Design,2016,16(6),3043—3048
[7] Cheng J.,Xu R.,Yang G.,J. Chem. Soc.,Dalton Trans.,1991,92(6),1537—1540
[8] Corma A.,Navarro M. T.,Rey F.,Rius J.,Navarro S. V.,Rey M. T.,Rius F.,Valencia J. S.,Angew. Chem. Int. Ed.,2001,40(12),2277—2280
[9] Corma A.,Navarro M. T.,Rey F.,Valencia S.,Chem. Commun.,2001,(18),1720—1721
[10] Kots P. A.,Sushkevich V. L.,Tyabikov O. A.,Ivanova I. I.,Micro. Meso. Mater.,2017,243,186—192
[11] Liu X.,Chu Y.,Wang Q.,Wang W.,Wang C.,Xu J.,Deng F.,Solid State Nuclear Magnetic Resonance,2017,87,1—9
[12] Liu D. R.,Gao Z. H.,Zi W. W.,Zhang J.,Du H. B.,Chen F. J.,Micro. Meso. Mater.,2019,276,232—238
[13] Liu X.,Xu H.,Zhang L.,Han L.,Jiang J.,Oleynikov P.,Chen L.,Wu P.,ACS Catal.,2016,6(12),8420—8431
[14] Bai R.,Sun Q.,Wang N.,Zou Y.,Guo G.,Iborra S.,Corma A.,Yu J.,Chem. Mater.,2016,28(18),6455—6458
[15] Tang L.,Shi L.,Bonneau C.,Sun J.,Yue H.,Ojuva A.,Lee B. L.,Kritikos M.,Bell R. G.,Bacsik Z.,Nat. Mater.,2008,7(5),381—385
[16] Rojas A.,Arteaga O.,Kahr B.,Camblor M. A.,J. Am. Chem. Soc.,2013,135(32),11975—11984
[17] Zhang N.,Shi L.,Yu T.,Li T.,Hua W.,Lin C.,J. Solid State Chem.,2015,225,271—277
[18] Shi L.,Yu T. T.,Lin S.,Yuan Y. B.,Wang J. K.,Zhang N.,Chem. J. Chinese Universities,2015,36(8),1467—1471(石磊,于婷婷,林森,袁玉斌,王济凯,张娜.高等学校化学学报,2015,36(8),1467—1471)
[19] Moeller K.,Yilmaz B.,Jacubinas R. M.,Mueller U.,Bein T.,J. Am. Chem. Soc.,2011,133(14),5284—5295
[20] Kubu M.,Millini R.,ilkováN.,Catal. Today,2019,324,3—14
[21] Jabri H. A.,Miyake K.,Ono K.,Nakai M.,Hirota Y.,Uchida Y.,Miyamoto M.,Nishiyama N.,Micro. Meso. Mater.,2019,278,322—326
[22] Zheng J.,Lin D.,Liu Z.,Zhu K.,Zhou X.,Yuan W.,Ind. Eng. Chem. Res.,2018,57(2),548—558
[23] Rimaz S.,Halladj R.,Askari S.,J. Colloid Inter. Sci.,2016,464,137—146
[24] Zhou D.,Lu X.,Xu J.,Yu A.,Li J.,Deng F.,Xia Q.,Chem. Mater.,2012,24(21),4160—4165
[25] Neumann G. T.,Hicks J. C.,Cryst. Growth Des.,2013,13(4)1535—1542
[26] Chen Y.,Li C.,Wang L.,Zhang M.,Liang C.,Micro. Meso. Mater.,2017,252,146—153
[27] Velaga B.,Peela N. R.,Micro. Meso. Mater.,2019,279,211—219
[28] Shi L.,Wang J.,Li N.,Lin S.,J. Alloys Compounds,2017,695,2488—2498
[29] Shi L.,Wang J.,Lin S.,Sun J.,Mater. Lett.,2017,186,382—385
[30] Cheng X.,Mao J.,Lv X.,Hua T.,Cheng X.,Long Y.,Tang Y.,J. Mater. Chem. A,2014,2(5),1247—1251
[31] Zhang L.,Huang Y.,J. Phys. Chem. C,2016,120(45),25945—25957
[32] Du Q.,Guo Y.,Wu P.,Liu H.,Micro. Meso. Mater.,2018,264,272—280
[33] Rao P. R. H. P.,Matsukata M.,Chem. Commun.,1996,(12),1441—1442
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