利用紫外共振拉曼光谱和紫外-可见漫反射光谱对不同铁含量的FeAlPO4-5分子筛进行了研究.结果表明,FeAlPO4-5分子筛的骨架铁有4个特征的拉曼谱峰,分别位于630,1060,1140和1210 cm-1.当凝胶中A1/Fe比小于380时,只有一部分铁离子可以进入分子筛形成四配位的骨架铁物种;而另一部分则以骨架外六配位的铁物种存在,其特征拉曼谱峰位于285 cm-1.结合紫外拉曼光谱、紫外-可见漫反射光谱和X射线衍射研究了Al/Fe比为760时FeAlPO4-5分子筛的晶化过程.结果发现,在分子筛晶化前,铁物种以六配位的形式存在,它为分子筛前体中的一维链状磷酸铝添加了一个惰性端基,六配位的Fe-O键不利于它与其它磷酸铝物种发生反应;当分子筛开始晶化时,带有铁离子端基的磷酸铝链与其它磷酸铝链进一步反应形成分子筛骨架.同时,六配位的铁离子和邻近的磷酸铝物种反应转化为四配位的骨架铁物种.
参考文献
[1] | Wilson S T;Lok B M;Messina C A;Cannan T R Flanigen E M .[J].Journal of the American Chemical Society,1982,104:1146. |
[2] | Jia J F;Wen B;Sachtler W M H .[J].Journal of Catalysis,2002,210:453. |
[3] | Joyner R;Stockenhuber M .[J].Journal of Physical Chemistry B,1999,103:5963. |
[4] | Lobree L J;Hwang I C;Reimer J A;Bell A T .[J].Journal of Catalysis,1999,186:242. |
[5] | Marturano P.;Kogelbauer A.;Prins R.;Drozdova L. .Fe/ZSM-5 prepared by sublimation of FeCl3: The structure of the Fe species as determined by IR, Al-27 MAS NMR, and EXAFS spectroscopy[J].Journal of Catalysis,2000(1):236-247. |
[6] | Sun K;Xia H;Feng Z;van Santen R Hensen E Li C .[J].Journal of Catalysis,2008,254:383. |
[7] | Sun KQ;Xia H;Hensen E;van Santen R;Li C .Chemistry of N2O decomposition on active sites with different nature: Effect of high-temperature treatment of Fe/ZSM-5[J].Journal of Catalysis,2006(1):186-195. |
[8] | 赵晓旭,程党国,陈丰秋,詹晓力.Fe含量对FeAlPO-5催化剂上甲烷还原N_2O反应的影响[J].催化学报,2010(01):68-71. |
[9] | Ren T;Yan L;Zhang X M;Suo J S .[J].Applied Catalysis A:General,2003,244:11. |
[10] | Raja R;Sankar G;Thomas J M .[J].Journal of the American Chemical Society,1999,121:11926. |
[11] | Dugal M.;Raja R.;Thomas JM.;Sankar G. .Designing a heterogeneous catalyst for the production of adipic acid by aerial oxidation of cyclohexane[J].Angewandte Chemie International Edition,2000(13):2310-2313. |
[12] | Shiju NR;Fiddy S;Sonntag O;Stockenhuber M;Sankar G .Selective oxidation of benzene to phenol over FeAlPO catalysts using nitrous oxide as oxidant[J].Chemical communications,2006(47):4955-4957. |
[13] | Wei W;Moulijn J A;Mul G .[J].Microporous and Mesoporous Materials,2008,112:193. |
[14] | Fan WB;Duan RG;Yokoi T;Wu P;Kubota Y;Tatsumi T .Synthesis, crystallization mechanism, and catalytic properties of titanium-rich TS-1 free of extraframework titanium species[J].Journal of the American Chemical Society,2008(31):10150-10164. |
[15] | Dutta P K;Bronic J .[J].Zeolites,1994,14:250. |
[16] | Dutta P K;Shieh D C;Puri M .[J].Journal of Physical Chemistry,1987,91:2332. |
[17] | Li C. .UV Resonance Raman Spectroscopic Identification of Titanium Atioms in the Framework of TS-1 Zeolite[J].Angewandte Chemie International Edition,1999(15):2220-2222. |
[18] | Li C. .Identifying the isolated transition metal ions/oxides in molecular sieves and on oxide supports by UV resonance Raman spectroscopy[J].Journal of Catalysis,2003(1/2):203-212. |
[19] | Fan F T;Sun K J;Feng Z C;Xia H A Han B Lian Y X Ying P L Li C .[J].Chemistry-A European Journal,2009,15:3268. |
[20] | 范峰滔,徐倩,夏海岸,孙科举,冯兆池,李灿.催化材料的紫外拉曼光谱研究[J].催化学报,2009(08):717-739. |
[21] | Fan F T;Feng Z C;Li C .[J].Accounts of Chemical Research,2010,43:378. |
[22] | Fan F T;Feng Z C;Li C .[J].Chemical Society Reviews,2010,39:4794. |
[23] | Li C .[J].Studies in Surface Science and Catalysis,2007,170:561. |
[24] | Li C;Xiong G;Liu J K;Ying P L Xin Q Feng Z C .[J].Journal of Physical Chemistry B,2001,105:2993. |
[25] | Fan F T;Feng Z C;Sun K J;Guo M L,Guo Q,Song Y,Li W X,Li C .[J].Angewandte Chemie International Edition,2009,48:8743. |
[26] | Sun K J;Fan F T;Xia H A;Feng Z C Li W X Li C .[J].Journal of Physical Chemistry C,2008,112:16036. |
[27] | 孙科举 .[D].大连:中国科学院大连化学物理研究所,2009. |
[28] | Li L X;Tang X C;Liu H T;Qu Y Lu Z G .[J].Electrochimica Acta,2010,56:995. |
[29] | Grandjean D;Beale A M;Petukhov A V;Weckhuysen B M .[J].Journal of the American Chemical Society,2005,127:14454. |
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:
-
10%
-
20%
-
30%
-
40%
-
50%