以十六烷基三甲基溴化铵(CTMAB)为模板剂,合成出Zr-FSM-16中孔分子筛,并采用XRD,IR和BET等对分子筛进行了表征. 考察了Zr掺杂量和pH值等因素对分子筛结构的影响,并考察了合成出的Zr-FSM-16分子筛对苯羟基化反应的催化性能. 结果表明,Zr能有效地嵌入FSM-16的骨架之中,但Zr的嵌入对分子筛中孔结构的形成具有一定的不利影响,随着Zr嵌入量的增加,分子筛的长程有序度会下降; pH值对分子筛中孔结构的形成也具有十分显著的影响,在n(Si)/n(Zr)=40的条件下, pH＜12.5时,有序度随着pH值的升高而升高,pH＞12.5时则相反. 一般在n(Si)/n(Zr)＞40时,催化剂均能保持较好的六方晶体结构和较大的比表面积; n(Si)/n(Zr)＜20时,则较难形成中孔结构. Zr-FSM-16对于苯的羟基化反应具有良好的催化性能,催化活性和选择性均随Zr嵌入量的增加而升高,n(Si)/n(Zr)=40时,苯酚的选择性可达65%以上.
参考文献
| [1] | Yanagisawa T;Shimizu T;Kuroda K;Kato C .[J].Bulletin of the Chemical Society of Japan,1990,63(04):988. |
| [2] | Inagaki S;Koiwai A;Suzuki N;Fukushima Y, Kuroda K .[J].Bulletin of the Chemical Society of Japan,1996,69(05):1449. |
| [3] | Fukuoka A;Osada M;Shido T;Inagaki S,Fukushima Y,Ichikawa M .[J].Inorganica Chimica Acta,1999,294(02):281. |
| [4] | Chatterjee M;Iwasaki T;Onodera Y;Hayashi H, Ikushima Y, Nagase T, Ebina T .[J].Applied Clay Science,2004,25(3/4):195. |
| [5] | Horniakova J;Raja T;Kubota Y;Sugi Y .[J].Journal of Molecular Catalysis A:Chemical,2004,217(1/2):73. |
| [6] | Mohamed M M;Eissa N A .[J].Materials Research Bulletin,2003,38(15):1993. |
| [7] | Sakamoto Y;Fukuoka A;Higuchi T;Shimomura N, Inagaki S, Ichikawa M .[J].Journal of Physical Chemistry B,2004,108(03):853. |
| [8] | Dhepe PL.;Fukuoka A.;Ichikawa M. .Novel fabrication and catalysis of nano-structured Rh and RhPt alloy particles occluded in ordered mesoporous silica templates using supercritical carbon dioxide[J].Physical chemistry chemical physics: PCCP,2003(24):5565-5573. |
| [9] | Matsuhashi H;Tanaka M;Nakamura H;Arata K .[J].Applied Catalysis A:General,2001,208(1/2):1. |
| [10] | Bianchi AO.;Maireles-Torres P.;Castellon ER.;Lopez AJ. Vaccari A.;Campanati M. .Si/Zr mesoporous catalysts for the vapour phase synthesis of alkylindoles[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2001(1/2):105-112. |
| [11] | Occelli M L;Biz S;Auroux A .[J].Applied Catalysis A:General,1999,183(02):231. |
| [12] | 廖世军,季山,简弃非,王乐夫,Vladimir Linkov,Leslie Petrik.具有中孔结构的SO2-4/Zr-HMS型固体超强酸的合成和结构表征[J].高等学校化学学报,2003(03):469-472. |
| [13] | Inagaki S;Fukushima Y;Okada A;Kurauchi K,Kuroda K,Kato C.In: Proceedings of the Ninth International Zeolite Conference[J].Canada Montreal,1992:305. |
| [14] | Szostak R.Molecular Sieves: Principles of Synthesis, and Identification[M].New York: Van Norstrand,1989:316. |
| [15] | Kostova N G;Spojakina A A;Jiratova K;Solcova O,Dimitrov L D,Petrov L A .[J].Catalysis Today,2001,65(2-4):217. |
| [16] | 王丽琴,王祥生,郭新闻,李钢,修景海,刘松.合成TS-1分子筛的结晶动力学及催化性能研究[J].催化学报,2003(02):132-136. |
| [17] | 任瑜,钱林平,岳斌,贺鹤勇.对环氧化反应具有高催化活性的钛硅介孔分子筛的制备[J].催化学报,2003(12):947-950. |
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%