采用完全液相法,分别以无机和有机Al源和Zr源制备了3个Cu-Zn-Al-Zr浆状催化剂,并采用X射线衍射、X射线光电子能谱和程序升温还原等手段对催化剂进行了表征,考察了催化剂在合成气一步法合成二甲醚反应中的催化性能.结果表明,不同Al源对催化剂的性能有显著影响,而不同Zr源对催化剂性能的影响不大.以异丙醇铝为原料制备的催化剂的活性明显高于以拟薄水铝石为原料制备的催化剂.以异丙醇铝为Al源制备的催化剂,其Cu组分粒度小、分散性好,Cu-Zr之间的相互作用较强.Al源中微量杂质Na的存在和Cu-Zr之间相互作用的强弱是导致催化剂性能差异的主要原因.
Cu-Zn-Al-Zr slurry catalyst samples were prepared from different raw materials of Al and Zr by a complete liquid-phase technol- ogy and characterized by X-ray diffraction, X-ray photoelectron spectroscopy, and H_2 temperatare-programmed reduction. The catalytic performance of the samples for the direct synthesis of dimethyl ether from syngas was evaluated in a slurry reactor. The results indicated that different A1 raw materials influenced obviously the catalyst performance, while different Zr raw matecials had little effect on the catalyst performance. The activity of the catalyst samples with aluminum isopropoxide as the raw material was significantly higher than that with pseudo-boehmite. The catalyst samples with aluminum isopropoxide as the raw material had good Cu dispersion and strong interaction be-tween Cu and Zr. It was concluded that the existence of trace Na in AI raw materials and the strong interaction between Cu and Zr were the main reasons for good catalytic performance.
参考文献
[1] | 陈正华;牛玉琴 .[J].煤炭转化,1996,19(04):37. |
[2] | 谢克昌,李忠.煤基燃料的制备与应用[J].化工学报,2004(09):1393-1399. |
[3] | Wang Zh L;Wang J F;Diao J;Jin Y .[J].Chemical Engineering and Technology,2001,24:507. |
[4] | 王和平.合成气一步法制二甲醚工艺及催化剂研究进展[J].工业催化,2003(05):34-38. |
[5] | 谭猗生;解红娟;崔海涛;韩怡卓 钟炳 .[J].燃料化学学报,2005,33:602. |
[6] | Gao Zh H;Hao L F;Huang W;Xie K Ch .[J].Catalysis Letters,2005,102:139. |
[7] | 高志华,黄伟,郝利峰,谢克昌.浆态床用CuO/ZrO2催化剂的完全液相法合成及其对CO加氢的催化性能[J].催化学报,2006(01):86-90. |
[8] | 黄伟;高志华;郝利峰;阴丽华 谢克昌 .[P].CN 1613 560,2005. |
[9] | 高志华,黄伟,王将永,阴丽华,谢克昌.Cu-Zn-Al-Zr合成二甲醚浆状催化剂的完全液相制备及表征[J].化学学报,2008(03):295-300. |
[10] | 吴贵升;孙予罕;李永旺.[A].杭州:浙江大学出版社,2002 |
[11] | 孙鲲鹏,卢伟伟,邱凤炎,徐贤伦.ZrO2对合成二甲醚双功能催化剂表面结构及催化性能的影响[J].分子催化,2003(03):168-172. |
[12] | 刘宏伟,聂兆广,刘殿华,应卫勇,房鼎业.三相淤浆床中合成气直接合成二甲醚双功能混合催化剂的失活研究[J].华东理工大学学报(自然科学版),2006(04):365-369,380. |
[13] | 吴茨萍;刘姝;穆文俊;王志娟 吴亚勤 贺立敏 .[J].抚顺石油学院学报,2000,20(07) |
[14] | 左宜赞;安欣;韩明汉;王金福 王德峥 金涌 .[J].催化学报,2008,29:166. |
[15] | 刘志坚,廖建军,谭经品,李大东.甲醇脱水生成二甲醚的沸石催化剂[J].石油化工,1999(04):236-239. |
[16] | Jun K W;Shen W J;Rao K S R;Lee K W .[J].Applied Catalysis A:General,1998,174:231. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%