对比研究了SSZ-13(CHA拓扑结构)和RUB-50(LEV拓扑结构)硅铝分子筛笼大小对甲醇制烯烃反应性能的影响,并采用X射线衍射、N2吸附-脱附、固体核磁共振、热重和紫外-可见光谱等技术对催化剂的结构及反应后的碳物种进行了表征.结果表明,笼尺寸较大的SSZ-13分子筛在反应中的稳定性和产物丙烯选择性均较高;而笼尺寸较小的RUB-50分子筛中乙烯的选择性较高.酸洗可以除去分子筛中大部分非骨架Al,且在一定程度上改变了分子筛的酸性,但没有显著改变产物中乙烯和丙烯的相对比例.另外,分子筛笼的大小决定了碳物种的体积,较小笼径的分子筛上可能生成较多的乙烯.因此,用于甲醇制烯烃的分子筛笼径大小对调变产物中乙烯和丙烯选择性十分重要.
参考文献
[1] | Stocker M .[J].Microporous and Mesoporous Materials,1999,29:3. |
[2] | Keil F J .[J].Microporous and Mesoporous Materials,1999,29:49. |
[3] | Liu Z M;Liang J .[J].Current Opinion in Solid State and Materials Science,1999,4:80. |
[4] | Inui T;Phatanasri S;Matsuda H.[J].Journal of the Chemical Society,Chemical Communications,1990:205. |
[5] | Inoue M;Dhupatemiya P;Phatanasri S;Inui T .[J].Microporous and Mesoporous Materials,1999,28:19. |
[6] | Zhao T S;Takemoto T;Tsubaki N .[J].Catalyst Communication,2006,7:647. |
[7] | Liu J;Zhang C X;Shen Z H;Hua W M Tang Y Shen W Yue Y H Xu H L .[J].Catalyst Communication,2009,10:1506. |
[8] | Li P;Zhang W P;Han X W;Bao X H .[J].Catalysis Letters,2010,134:124. |
[9] | 郭强胜,毛东森,劳嫣萍,卢冠忠.氟改性对纳米HZSM-5分子筛催化甲醇制丙烯的影响[J].催化学报,2009(12):1248-1254. |
[10] | Mei CS;Wen PY;Liu ZC;Liu HX;Wang YD;Yang WM;Xie ZK;Hua WM;Gao Z .Selective production of propylene from methanol: Mesoporosity development in high silica HZSM-5[J].Journal of Catalysis,2008(1):243-249. |
[11] | Sun, C;Du, JM;Liu, J;Yang, YS;Ren, N;Shen, W;Xu, HL;Tang, Y .A facile route to synthesize endurable mesopore containing ZSM-5 catalyst for methanol to propylene reaction[J].Chemical communications,2010(15):2671-2673. |
[12] | Song W G;Fu H;Haw J F .[J].Journal of the American Chemical Society,2001,123:4749. |
[13] | Yamamoto K;Ikeda T;Onodera M;Muramatsu A Mizukami F Wang Y Gies H .[J].Microporous and Mesoporous Materials,2010,128:150. |
[14] | Park J W;Lee J Y;Kim K S;Hong S B Seo G .[J].Applied Catalysis A:General,2008,339:36. |
[15] | Li X J;Zhang W P;Liu S L;Xu L Y Han X W Bao X H .[J].Journal of Catalysis,2007,250:55. |
[16] | Fyfe C A;Feng Y;Grondey H;Kokotailo G T Gies H .[J].Chemical Reviews,1991,91:1525. |
[17] | 刘勇,张维萍,谢素娟,徐龙伢,韩秀文,包信和.用固体核磁共振研究HZSM-35分子筛的酸性[J].催化学报,2009(02):119-123. |
[18] | Zhu Q J;Kondo J N;Ohnuma R;Kubota Y Yamaguchi M Tatsumi T .[J].Microporous and Mesoporous Materials,2008,112:153. |
[19] | Song W G;Haw J F .[J].Angewandte Chemie International Edition,2003,42:892. |
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%