Zr0.5Ti0.5O2的添加对超临界裂解RP-3催化剂性能的影响

doi:10.3866/PKU.WHXB201308271

物理化学学报 >> 2013, Vol. 29 >> Issue (10): 2255-2262.doi: 10.3866/PKU.WHXB201308271

Zr_0.5Ti_0.5O₂的添加对超临界裂解RP-3催化剂性能的影响

焦毅¹, 秦莉晓², 李雄健², 王佳², 王健礼¹, 朱权², 李象远², 陈耀强¹

1 四川大学化学学院, 绿色化学与技术教育部重点实验室, 成都 610064;
2 四川大学化工学院, 成都 610064

收稿日期:2013-06-18 修回日期:2013-08-26 发布日期:2013-09-26
通讯作者: 王健礼 E-mail:wangjianli@scu.edu.cn
基金资助:
国家自然科学基金(91016002);四川大学优秀青年学者科研基金(2013SCU04A05);国家高技术研究发展计划项目(863)(2006AA01A119)和高超声速冲压发动机技术重点实验室开放基金(20120103013)资助

Influence of Adding Zr_0.5Ti_0.5O₂ on the Performance of Supercritical Cracking Catalyst for RP-3

JIAO Yi¹, QIN Li-Xiao², LI Xiong-Jian², WANG Jia², WANG Jian-Li¹, ZHU Quan², LI Xiang-Yuan², CHEN Yao-Qiang¹

1 Key Laboratory of Green Chemistry and Technology of the Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China;
2 College of Chemical Engineering, Sichuan University, Chengdu 610064, P. R. China

Received:2013-06-18 Revised:2013-08-26 Published:2013-09-26
Contact: WANG Jian-Li E-mail:wangjianli@scu.edu.cn
Supported by:
The project was supported by the National Natural Science Foundation of China (91016002), Outstanding Young Scholar Fund of Sichuan University, China (2013SCU04A05), National High-Tech Research and Development Program of China (863) (2006AA01A119), and Open Foundation of Key Laboratory on Hypersonic Scramjet Technology, China (20120103013).

摘要/Abstract

摘要：

采用共沉淀法制备了Zr_0.5Ti_0.5O₂载体材料,将其掺杂在CeO₂-Al₂O₃ (CA)基催化剂中, 并对其催化活性进行了超临界裂解测试, 采用全自动吸附仪、X射线衍射(XRD)、透射电镜(TEM)、程序升温脱附(TPD)等方法对催化剂进行了表征. 实验结果表明, 催化剂能够明显降低裂解反应的温度, 600 ℃ CA基催化剂产气率是热裂解的2.8倍, 掺杂Zr_0.5Ti_0.5O₂载体材料的CA基催化剂是热裂解的4.0倍, 650 ℃时, 掺杂Zr_0.5Ti_0.5O₂载体材料的CA基催化剂热沉提高了0.55 MJ·kg^-1. BET结果表明, 掺杂Zr_0.5Ti_0.5O₂载体后催化剂出现双孔结构, 部分小孔的出现使得乙烯的选择性提高; NH₃-TPD结果表明, 掺杂Zr_0.5Ti_0.5O₂载体材料后, 催化剂强酸位的酸量增加了4.0倍,催化剂表现出更强的表面酸性和更集中的强酸酸中心密度, 有利于裂解多产烯烃.

关键词: 吸热燃料, 钛锆复合氧化物, 超临界, 催化裂解, 热沉

Abstract:

Zr_0.5Ti_0.5O₂ was prepared by co-precipitation and tested for its catalytic performance under supercritical conditions when mixed with a CeO₂-Al₂O₃ (CA) base catalyst. The catalysts were characterized with an automatic adsorption instrument (BET method), X-ray diffraction (XRD), transmission electron microscopy (TEM), and temperature programmed desorption (TPD). It was found that Zr_0.5Ti_0.5O₂ significantly lowered the temperature of the cracking reaction, and increased the thermal cracking gas rate by a factor of 2.8 times as large as that at 600 ℃ for the CAbase catalyst. The gas rate was increased by a factor of 4.0 times when it was doped into the CAbase catalyst, and the heat sink increased by 0.55 MJ·kg^-1 over that of thermal cracking at 650 ℃. BET results show that the Zr_0.5Ti_0.5O₂-doped CAbase catalyst has a double-pore structure that enhances ethylene selectivity. NH3-TPD result indicates that the acidity of the catalyst increased by 4.0 times, indicating improved surface acidity conducive to alkene generation.

Key words: Endothermic fuel, ZrO₂-TiO₂ composite oxide, Supercritical, Catalytic cracking, Heat sink

MSC2000:

O643.36

焦毅, 秦莉晓, 李雄健, 王佳, 王健礼, 朱权, 李象远, 陈耀强. Zr_0.5Ti_0.5O₂的添加对超临界裂解RP-3催化剂性能的影响[J]. 物理化学学报, 2013, 29(10): 2255-2262.

JIAO Yi, QIN Li-Xiao, LI Xiong-Jian, WANG Jia, WANG Jian-Li, ZHU Quan, LI Xiang-Yuan, CHEN Yao-Qiang. Influence of Adding Zr_0.5Ti_0.5O₂ on the Performance of Supercritical Cracking Catalyst for RP-3[J]. Acta Phys. -Chim. Sin., 2013, 29(10): 2255-2262.

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Zr_0.5Ti_0.5O₂的添加对超临界裂解RP-3催化剂性能的影响

Influence of Adding Zr_0.5Ti_0.5O₂ on the Performance of Supercritical Cracking Catalyst for RP-3

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