欢迎登录材料期刊网

材料期刊网

高级检索

以四乙基氢氧化铵为有机结构导向剂,采用超浓水热方法,从氟离子体系合成出手性多形体A(简称A形体)富集的全硅beta沸石。在同样的初始混合物中引入铝源后,所合成的beta沸石中A形体含量明显降低,产物为普通的硅铝beta沸石。用粉末X射线衍射、元素分析、热重-差热分析、氮气吸附、扫描电子显微镜和固体魔角自旋核磁共振等表征手段对全硅beta沸石和硅铝beta沸石进行了详细的表征,并研究了其晶化过程。结果表明,铝源的引入可以加速beta沸石的晶化,得到的硅铝beta沸石晶体粒径明显减小。在硅铝beta沸石的晶化过程中生成了五配位铝物种,五配位铝物种可能是导致产物中A形体含量降低的原因。

Using tetraethylammonium hydroxide as the organic structure-directing agent and in the presence of fluoride, polymorph A-enriched silica beta zeolite was synthesized under concentrated hydro-thermal conditions. The introduction of Al species into the same starting mixture resulted in a de-crease in the degree of enrichment of polymorph A in beta zeolite and an Al-incorporated beta zeo-lite resulted. The crystallized polymorph A-enriched silica beta zeolite and the Al-incorporated beta zeolite and their crystallization processes were investigated by X-ray diffractometry, elemental analysis, thermogravimetric analysis-differential thermal analysis, nitrogen adsorption, scanning electron microscopy, and solid-state magic angle spinning nuclear magnetic resonance. The intro-duction of Al species accelerated crystallization and reduced the crystal size of Al-incorporated beta zeolite. The intermediate of five-coordinated Al species accounted for a decrease in the degree of enrichment of polymorph A in the crystallization of Al-incorporated beta zeolite.

参考文献

[1] Wadlinger R L;Kerr G T;Rosinski E J .[P].US Patent 3 308 069,1967.
[2] Newsam J M;Treacy M M J;Koetsier W T;De Gruyter C B .[J].Proceedings of the Royal Society of London Series A:Mathematical and Physical Sciences,1988,420:375.
[3] Higgins J B;LaPierre R B;Schlenker J L;Rohrman A C Wood J D Kerr G T Rohrbaugh W J .[J].ZEOLITES,1988,8:446.
[4] Davis M E;Lobo R F .[J].CHEMISTRY OF MATERIALS,1992,4:756.
[5] Camblor M A;Corma A;Valencia S.[J].Chemistry Communications,1996:2365.
[6] Xia Q H;Shen S C;Song J;Kawi S Hidajat K .[J].Journal of Catalysis,2003,219:74.
[7] Takagi Y;Komatsu T;Kitabata Y .[J].Microporous and Mesoporous Materials,2008,109:567.
[8] Taborda F;Willhammar T;Wang Z Y;Montes C Zou X D .[J].Mi-croporous Mesoporous Mater,2011,143:196.
[9] 童明全,闫文付,于吉红,徐如人.A形体过量β沸石的晶化过程[J].高等学校化学学报,2013(03):494-498.
[10] 郭文,闫文付,徐如人,王永睿,慕旭宏.以两种季铵碱为模板剂合成A形体富集Beta沸石及其晶化过程[J].高等学校化学学报,2014(07):1363-1368.
[11] Camblor M A;Corma A;Martinez A;Perez-Pariente J.[J].Journal of the Chemical Society,Chemical Communications,1992:589.
[12] Corma A;Nemeth L T;Renz M;Valencia S .[J].NATURE,2001,412:423.
[13] Jin J J;Ye X X;Li Y S;Wang Y Q Li L Gu J L Zhao W R Shi J L .[J].DALTON TRANSACTIONS,2014,43:8196.
[14] Li Y J;Armor J N.[J].Chemistry Communications,1997:2013.
[15] Santi D;Holl T;Calemma V;Weitkamp J .[J].Applied Catalysis A:General,2013,455:46.
[16] Zhu YZ;Chuah G;Jaenicke S .Chemo- and regioselective Meerwein-Ponndorf-Verley and Oppenauer reactions catalyzed by Al-free Zr-zeolite beta[J].Journal of Catalysis,2004(1):1-10.
[17] Hazm J E;Caullet P;Paillaud J L;Soulard M Delmotte L .[J].Mi-croporous Mesoporous Mater,2001,43:11.
[18] Bourgeat-Lami E;Di Renzo F;Fajula F;Mutin P H Des Courieres T .[J].Journal of Physical Chemistry,1992,96:3807.
[19] Camblor M A;Corma A;Valencia S .[J].Microporous and Mesoporous Materials,1998,25:59.
[20] Serrano D P;Van Grieken R;Sanchez P;Sanz R Rodriguez L .[J].Mi-croporous Mesoporous Mater,2001,46:35.
[21] Camblor MA.;Valencia S.;Corma A. .Synthesis in fluoride media and characterisation of aluminosilicate zeolite beta[J].Journal of Materials Chemistry: An Interdisciplinary Journal dealing with Synthesis, Structures, Properties and Applications of Materials, Particulary Those Associated with Advanced Technology,1998(9):2137-2145.
[22] Hartmeyer G;Marichal C;Lebeau B;Caullet P;Hernandez J .Fluorination of silica nanoparticles by aqueous NH4F solutions[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2007(18):6634-6644.
[23] Harris R K;Newman R H;J Chem Soc .[J].Faraday Trans 2,1977,73:1204.
上一张 下一张
上一张 下一张
计量
  • 下载量()
  • 访问量()
文章评分
  • 您的评分:
  • 1
    0%
  • 2
    0%
  • 3
    0%
  • 4
    0%
  • 5
    0%