超声波碱处理改性对丝光沸石结构、酸性质及其催化性能的影响

doi:10.11949/j.issn.0438-1157.20171632

化工学报 ›› 2018, Vol. 69 ›› Issue (7): 3001-3008.DOI: 10.11949/j.issn.0438-1157.20171632

• 催化、动力学与反应器 • 上一篇下一篇

超声波碱处理改性对丝光沸石结构、酸性质及其催化性能的影响

韩海波^1,2, 王有和¹, 李康², 刘丹禾², 郝代军², 阎子峰¹

1 中国石油大学重质油国家重点实验室, 山东青岛 266580;
2中石化炼化工程集团洛阳技术研发中心, 河南洛阳 471003

收稿日期:2017-12-12 修回日期:2018-01-31 出版日期:2018-07-05 发布日期:2018-07-05
通讯作者: 阎子峰
基金资助:
国家自然科学基金项目（21776311）；中央高校基本科研业务费专项资金项目（15CX05030A）。

Effect of ultrasonic alkali treatment on structural, acidic properties and performance of MOR catalyst

HAN Haibo^1,2, WANG Youhe¹, LI Kang², LIU Danhe², HAO Daijun², YAN Zifeng¹

1 State Key Laboratory for Heavy Oil Processing, China University of Petroleum, Qingdao 266580, Shandong, China;
2 Luoyang R & D Center of Technology of Sinopec Engineering(Group) CO., LTD., Luoyang 471003, Henan, China

Received:2017-12-12 Revised:2018-01-31 Online:2018-07-05 Published:2018-07-05
Supported by:
supported by the National Natural Science Foundation of China(21776311) and the Fundamental Research Funds for the Central Universities (15CX05030A).

摘要/Abstract

摘要：

基于丝光沸石（MOR）催化合成乙酸甲酯稳定性较差及传统碱处理MOR较难引入多级孔的特性，提出了利用超声波对MOR进行碱处理脱硅改性以制备多级孔MOR的技术。采用XRD、SEM、TEM、吡啶红外和N₂吸-脱附等手段对催化剂进行了表征，分别考察了超声波在不同碱浓度处理改性条件下对分子筛催化剂骨架结构、酸性质、孔结构以及催化合成乙酸甲酯性能的影响。结果表明，通过超声波及合适浓度的NaOH碱溶液处理后，MOR分子筛的酸量、介孔孔容、比表面积都增加、孔径分布变宽，催化剂的活性和稳定性等催化性能得以改善。改性后的MOR催化剂二甲醚（DME）转化率由35.3%增加到44.8%，使用寿命大大延长，但碱液浓度过高会严重破坏MOR分子筛骨架结构，催化活性及稳定性快速下降。

关键词: 超声波, 碱处理改性, DME羰基化, 多级孔MOR

Abstract:

MOR catalyst commonly suffers the poor stability in the catalytic synthesis of methyl acetate. It's difficulty to introduce the hierarchical pores by traditional alkali treatment. To overcome this drawback, an ultrasonic alkali treatment was utilized to generate hierarchical MOR via desilication. Multiple analyzing methods, such as XRD, SEM, TEM, pyridine IR and N₂ adsorption-desorption, were used to characterize the catalyst structure and the influence of ultrasonic treatment under different alkali concentration on the MOR framework. Acidity, pore structure and catalytic properties were investigated. The results showed that a proper ultrasonic alkali treatment could significantly improve the number of acidic sites, mesopore volume, surface area, pore size distribution, catalytic activity and stability. The DME conversion increased from 35.3% to 44.8%, and the catalyst lifetime was greatly prolonged. However, an excessive alkali concentration seriously destroyed the MOR framework, leading to a rapid decrease on catalyst activity and stability.

Key words: ultrasonic, alkali treatment, DME carbonylation, hierarchical MOR

中图分类号:

O643

韩海波, 王有和, 李康, 刘丹禾, 郝代军, 阎子峰. 超声波碱处理改性对丝光沸石结构、酸性质及其催化性能的影响[J]. 化工学报, 2018, 69(7): 3001-3008.

HAN Haibo, WANG Youhe, LI Kang, LIU Danhe, HAO Daijun, YAN Zifeng. Effect of ultrasonic alkali treatment on structural, acidic properties and performance of MOR catalyst[J]. CIESC Journal, 2018, 69(7): 3001-3008.

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超声波碱处理改性对丝光沸石结构、酸性质及其催化性能的影响

Effect of ultrasonic alkali treatment on structural, acidic properties and performance of MOR catalyst

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