预处理条件及金属离子改性对H-MOR分子筛的DME羰基化性能影响

doi:10.11949/j.issn.0438-1157.20150882

化工学报 ›› 2015, Vol. 66 ›› Issue (9): 3504-3510.DOI: 10.11949/j.issn.0438-1157.20150882

• 催化、动力学与反应器 • 上一篇下一篇

预处理条件及金属离子改性对H-MOR分子筛的DME羰基化性能影响

赵娜¹, 牛君阳¹, 刘亚华¹, 谭猗生², 李新刚¹

1 天津大学化工学院, 天津化学化工协同创新中心, 天津 300072;
2 中国科学院山西煤炭化学研究所, 煤转化国家重点实验室, 山西太原 030001

收稿日期:2015-06-10 修回日期:2015-06-30 出版日期:2015-09-05 发布日期:2015-09-05
通讯作者: 李新刚
基金资助:
国家自然科学基金项目(21476159);煤转化国家重点实验室开放课题(J15-16-902)。

Influence of pretreatment and metal cation modification of H-MOR zeolite on performance of DME carbonylation

ZHAO Na¹, NIU Junyang¹, LIU Yahua¹, TAN Yisheng², LI Xingang¹

1 School of Chemical Engineering and Technology, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin University, Tianjin 300072, China;
2 State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Science, Taiyuan, 030001, Shanxi, China

Received:2015-06-10 Revised:2015-06-30 Online:2015-09-05 Published:2015-09-05
Supported by:
supported by the National Natural Science Foundation of China (21476159) and State Key Laboratory of Coal Conversion (J15-16-902).

摘要/Abstract

摘要：

详细了考察不同预处理条件及反应温度对丝光沸石(H-MOR)分子筛二甲醚(DME)羰基化制取醋酸甲酯(MA)的催化活性和稳定性的影响。研究结果表明,在氮气气氛中500℃预处理2 h、反应温度为180℃时H-MOR催化剂的DME转化率最高,可达20.5%。虽然提高反应温度可以进一步提高催化剂的DME转化率,但易产生积炭,快速失活。此外,还考察了金属离子改性对H-MOR催化剂DME羰基化活性的影响。采用离子交换法制备了Cu、Ni、Fe和Co等金属离子交换的H-MOR催化剂,活性测试结果表明:IE-Cu催化剂活性最好,DME转化率为36.9%;IE-Ni催化剂的活性最稳定,DME转化率稳定在24.5%。还原温度对IE-Cu催化剂DME羰基化活性有重要影响,450℃还原后的IE-Cu催化剂活性要明显高于300℃还原的IE-Cu。

关键词: 丝光沸石, 二甲醚, 羰基化, 金属离子改性

Abstract:

The influence of the pretreatment conditions and reaction temperature of the H-MOR zeolite on the performance of DME carbonylation was investigated. It was found that after the sample was pretreated in N₂ flow at 500℃ for 2 h, the DME conversion reached 20.5% at 180℃. The DME conversion of the H-MOR increased with increasing reaction temperature, but the serious coking at higher temperatures resulted in the deactivation of the catalyst. Additionally, Cu, Fe, Ni and Co cations were used to modify the H-MOR zeolite, and to explore the influence of metal cation modification of the H-MOR zeolite on the performance of DME carbonylation. The catalytic tests showed that the IE-Cu catalyst was more active with the DME conversion of 36.9%, while the IE-Ni catalyst was more stable with the DME conversion of around 24.5% at the whole reaction period. Moreover, the influence of reduction temperature of the IE-Cu zeolite on the performance of DME carbonylation was also studied. The catalytic activity of the pre-reduced IE-Cu at 450℃was higher than that pre-reduced at 300℃.

Key words: H-mordenite, dimethyl ether, carbonylation, metal cation modification

中图分类号:

赵娜, 牛君阳, 刘亚华, 谭猗生, 李新刚. 预处理条件及金属离子改性对H-MOR分子筛的DME羰基化性能影响[J]. 化工学报, 2015, 66(9): 3504-3510.

ZHAO Na, NIU Junyang, LIU Yahua, TAN Yisheng, LI Xingang. Influence of pretreatment and metal cation modification of H-MOR zeolite on performance of DME carbonylation[J]. CIESC Journal, 2015, 66(9): 3504-3510.

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预处理条件及金属离子改性对H-MOR分子筛的DME羰基化性能影响

Influence of pretreatment and metal cation modification of H-MOR zeolite on performance of DME carbonylation

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