利用一步水热合成法,在有机模板剂1,6-己二胺结构导向作用下,合成了具有MFI骨架结构的铁硅酸盐分子筛晶体Fe-Silicalite-1.并通过XRD、TG-DTA、IR和SEM等测试方法对其结构和性能进行了表征.ICP-AES及EDS分析结果表明:Fe原子进入到分子筛骨架上,质量分数约为0.66%.在以过氧化氢为氧化剂,羟化苯酚的催化反应中,苯酚的转化率为22.2%,其中65.8%为邻苯二酚,34.2%为对苯二酚.Fe-Silicalite-1分子筛晶体是一种良好的合成二酚的催化剂,具有潜在的应用价值.
Fe-Silicalite-1 zeolites with MFI framework structure were synthesized using 1,6-hexamethylene-diamine as a structure direction agent via one-step hydrothermal synthesis technique. The structure and properties of as-synthesized samples were characterized by XRD, SEM, IR, TG-DTA etc. EDS and ICP-AES indicated that the transition metal iron ions were framework elements and the mass fraction was 0.66%. The catalytic activity in hydroxylation of phenol with hydrogen peroxide as the oxidant was also investigated. The results showed that the phenol conversion is about 22.2%, and the selectivities of catechol and hydroquinone are 65.8% and 34.2% respectively. Fe-Silicalite-1 is a promising catalyst.
参考文献
| [1] | Taramasso M;Perogo G;Notari B .Preparation of Porous Crystalline Synthetic Materials Comprised of Silicon and Titanium Oxides[P].US Patent:4410501,1983. |
| [2] | 赵谦,殷广明,姜廷顺,殷恒波,唐雅静.水热条件下CuMCM-41介孔分子筛的合成与表征[J].硅酸盐学报,2007(05):619-623. |
| [3] | 马淑杰.双杂原子Ti-Fe-ZSM-5分子筛的合成与表征[J].高等学校化学学报,1997(04):504. |
| [4] | 高志贤;程昌瑞;谭长瑜 等.Na,NBA-Ga-Si-ZSM-5杂原子沸石分子筛的表征[J].催化学报,1996,17(06):556-558. |
| [5] | Jean-Philippe Tessonnier;Benoit Louis;Severinne Rigolet .Methane dehydro-aromatization on Mo/ZSM-5: About the hidden role of Bronsted acid sites[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2008(1/2):79-88. |
| [6] | Jin T;Hwang YK;Hong DY;Jhung SH;Hwang JS;Park SE;Kim YH;Chang JS .Microwave synthesis, characterization and catalytic properties of titanium-incorporated ZSM-5 zeolite[J].Research on Chemical Intermediates,2007(6):501-512. |
| [7] | Yang GH;He JJ;Yoneyama Y;Tan YS;Han YZ;Tsubaki N .Preparation, characterization and reaction performance of H-ZSM-5/cobalt/silica capsule catalysts with different sizes for direct synthesis of isoparaffins[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2007(0):99-105. |
| [8] | Piaoping Yang;Yongchen Shang;Jun Wang .EFFECT OF ACIDIC AND METALLIC SITES ON THE CATALYTIC PERFORMANCE OF Pd/ZSM-5 CATALYSTS IN THE ONE-STEPSYNTHESIS OF MIBK[J].Reaction kinetics & catalysis letters,2007(2):391-398. |
| [9] | Cl. T. Brigden;C. D. Williams;D. Apperley .A Study of the Chemistry of Isomorphous Substitution and Characterization of Al-ZSM-5 and Sc-ZSM-5 Synthesized in Fluoride Media[J].Inorganic materials,2007(7):758-769. |
| [10] | O. de la Iglesia;V. Sebastian;R. Mallada .Preparation of Pt/ZSM-5 films on stainless steel microreactors[J].Catalysis Today,2007(1/2):2-10. |
| [11] | K. Maduna Valkaj;A. Katovic;S. Zrncevic .Investigation of the catalytic wet peroxide oxidation of phenol over different types of Cu/ZSM-5 catalyst[J].Journal of hazardous materials,2007(3):663-667. |
| [12] | N.Rane;M.Kersbulck;R.A.van Santen;E.J.M.Hensen .Cracking of n-heptane over Bronsted acid sites and Lewis acid Ga sites in ZSM-5 zeolite[J].Microporous and mesoporous materials: The offical journal of the International Zeolite Association,2008(2/3):279-291. |
| [13] | 季东,任通,张小明,索继栓,丁勇.FeZSM-5/N2O催化氧化苯制苯酚[J].化学进展,2003(01):51-59. |
| [14] | Jifei Jia;Krishnan S.Pillai;Wolfgang M.H.Sachtler .One-step oxidation of benzene to phenol with nitrous oxide over Fe/MFI catalysts[J].Journal of Catalysis,2004(1):119-126. |
| [15] | 李哲,陈兵,黄伟,谢克昌.铁改性的Mo/ZSM-5催化剂上NO的选择性催化还原反应[J].高等学校化学学报,2006(10):1907-1911. |
| [16] | Mourad Mhamdi;Sihem Khaddar-Zine;Abdelhamid Ghorbel .Influence of the Co/Al ratio and the temperature of thermal treatment on cobalt speciation and catalytic properties of Co-ZSM-5 prepared by solid-state ion exchange[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2008(1):39-47. |
| [17] | Adalgisa Tavolaro;Palmira Tavolaro;Enrico Drioli .Influence of synthesis parameters on vanadium-silicalite-1 crystal growth prepared with fluoride-containing media[J].Journal of Crystal Growth,2006(2):609-616. |
| [18] | Cheng C H;Juttu G;Mitchell S F et al.Synthesis,Characterization,and Growth Rates of Germanium Silicalite-1 Grown from Clear Solutions[J].Journal of Physical Chemistry B,2006,110:21430-21437. |
| [19] | Milanesio M;Lamberti C;Aiello R et al.Iron Location in Fe-silicalites by Synchrotron Radiation Single Crystal X-ray Diffraction[J].Journal of Physical Chemistry B,2000,104:9951-9953. |
| [20] | Javier Perez-Ramirez;M.Santhosh Kumar;Angelika Bruckner .Reduction of N_2O with CO over FeMFI zeolites:influence of the preparation method on the iron species and catalytic behavior[J].Journal of Catalysis,2004(1):13-27. |
| [21] | Yihua Zhang;Daniel N.Briggs;Emiel de Smit .Effects of zeolite structure and composition on the synthesis of dimethyl carbonate by oxidative carbonylation of methanol on Cu-exchanged Y,ZSM-5,and Mordenite[J].Journal of Catalysis,2007(2):443-452. |
| [22] | Phiriyawirut P;Jamieson A M;Wongkasemjit S .VS-1 Zeolite Ssynthesized Directly from Silatrane[J].Microporous and Mesoporous Materials,2005,77:203-213. |
| [23] | Benjamin R.Wood;Jeffrey A.Reimer;Alexis T.Bell .Studies of N_2O Adsorption and Decomposition on Fe-ZSM-5[J].Journal of Catalysis,2002(1):151-158. |
| [24] | On DT.;Bonneviot L.;Kaliaguine S. .TITANIUM BORALITES WITH MFI STRUCTURE CHARACTERIZED USING XRD, XANES, IR, AND UV-VISIBLE TECHNIQUES - EFFECT OF HYDROGEN PEROXIDE ON THE PREPARATION[J].Journal of Catalysis,1995(1):235-243. |
| [25] | Yong Sig Ko;Hyun Tae Jang;Wha Seung Ahn .Hydrothermal Synthesis And Characterization Of Fe(iii)-substituted Mordenites[J].The Korean journal of chemical engineering,2008(6):1286-1291. |
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