分别用ZnSO4, Zn(AcO)2, Zn(NO3)2和ZnCl2溶液对HZSM-5分子筛浸渍改性得到不同Zn盐改性的HZSM-5催化剂。采用X射线衍射、N2物理吸附、热重-质谱分析、氨程序升温脱附和吡啶吸附红外光谱等方法对改性后的催化剂进行了表征,并在固定床反应装置上考察了其甲醇芳构化反应性能。结果表明,不同Zn盐改性的HZSM-5催化剂上Zn物种的存在形式不同会导致其表面酸中心强度与分布具有较大差异,经ZnSO4改性的HZSM-5催化剂表面上强B酸中心和Zn物种的存在使其表现出最佳的甲醇芳构化反应性能。
HZSM-5 catalysts modified with various Zn salts, namely zinc sulfate, zinc acetate, zinc nitrate, and zinc chloride, were prepared using an impregnation method. The resultant catalysts were charac-terized by X-ray diffraction, N2 adsorption, thermogravimetry-mass spectrometry, tempera-ture-programmed desorption of NH3, and infrared spectroscopy using pyridine as the probe mole-cule. The methanol-to-aromatic (MTA) performance over the modified catalysts was investigated. The results showed that the type of Zn species in the catalyst significantly influenced the catalyst surface acidity. The distribution of acid sites and Zn species in the HZSM-5 catalyst modified with zinc sulfate effectively improved the MTA performance.
参考文献
| [1] | 邹琥,吴巍,葸雷,朱宁,史军军.甲醇制芳烃研究进展[J].石油学报（石油加工）,2013(03):539-547. |
| [2] | Keil F J .[J].Microporous and Mesoporous Materials,1999,29:49. |
| [3] | St?cker M .[J].Microporous and Mesoporous Materials,1999,29:3. |
| [4] | Olsbye U;Svelle S;Bjorgen M;Beato P Janssens T V W Joensen F Bordiga S Lillerud K P .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2012,51:5810. |
| [5] | Cejka J;Van Bekkum H;Di Renzo F;Fajula F O.Zeolites and Ordered Mesoporous Materials:Progress and Prospects[M].Amsterdam:Elsevier,2005:380. |
| [6] | Chang C D;Silvestri A J .[J].Journal of Catalysis,1977,47:249. |
| [7] | Barthos R;Bansagi T;Zakar T S;Solymosi F .[J].Journal of Catalysis,2007,247:368. |
| [8] | Ono Y;Adachi H;Senoda Y .[J].Chem Soc Faraday Trans 1,1988,84:1091. |
| [9] | Jing H J;Yang F K;Xia Y M;Feng J Q Liu J L Zong Q Y .[J].PETROLEUM SCIENCE AND TECHNOLOGY,2012,30:1737. |
| [10] | Ni Y M;Sun A M;Wu X L;Hai G L Hu J L Li T Li G X .[J].Microporous and Mesoporous Materials,2011,143:435. |
| [11] | Zaidi H A;Pant K K .[J].Catalysis Today,2004,96:155. |
| [12] | Xin Y B;Qi P Y;Duan X P;Lin H Q Yuan Y Z .[J].Catalysis Letters,2013,143 |
| [13] | Song C;Liu K F;Zhang D Z;Liu S L Li X J Xie S J Xu L Y .[J].Applied Catalysis A:General,2014,470:15. |
| [14] | Lopez-Sanchez J A;Conte M;Landon P;Zhou W Bartley J K Taylor S H Carley A F Kiely C J Khalid K Hutchings G J .[J].Catalysis Letters,2012,142:1049. |
| [15] | Inoue Y;Nakashiro K;Ono Y .[J].Microporous Materials,1995,4:379. |
| [16] | Conte M;Lopez-Sanchez J A;He Q;Morgan D J Ryabenkova Y Bartley J K Carley A F Taylor S H Kiely C J Khalid K Hutchings G J .[J].Catal Sci Technol,2012,2:105. |
| [17] | 艾沙·努拉洪,刘家旭,贺宁,郭洪臣.正丁烷在Au,Zn组合改性纳米HZSM-5上的催化转化[J].催化学报,2013(06):1262-1266. |
| [18] | 佘励勤;王多才;李宣文;刘兴云 韩明 .[J].物理化学学报,1993,10:247. |
| [19] | 刘兴云;李宣文;佘励勤;袁世斌 秦皓昱 .[J].石油学报（石油加工）,1988,4(04):36. |
| [20] | Komatsu T.;Yashima T.;Mesuda M. .Aromatization of butane on Pt-Ge intermetallic compounds supported on HZSM-5[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2000(Special Issue SI):333-339. |
| [21] | Song Y Q;Zhu X X;Xu L Y .[J].CATALYSIS COMMUNICATIONS,2006,7:218. |
| [22] | 田涛,骞伟中,汤效平,恽松,魏飞.甲醇芳构化反应中Ag/ZSM-5催化剂的失活特性[J].物理化学学报,2010(12):3305-3309. |
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