双亲型Ti/ZSM-5分子筛催化剂的制备及氧化脱硫性能

doi:10.7503/cjcu20180770

高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (6): 1265.doi: 10.7503/cjcu20180770

双亲型Ti/ZSM-5分子筛催化剂的制备及氧化脱硫性能

王影², 孙传胤¹, 王润伟¹, 张震东¹(), 张大明², 张宗弢¹(), 裘式纶¹

1. 吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春130012
2. 吉林大学电子科学与工程学院, 集成光电子学国家重点联合实验室, 长春 130012

收稿日期:2018-11-15 出版日期:2019-06-10 发布日期:2019-04-04
作者简介:联系人简介: 张宗弢, 男, 博士, 教授, 博士生导师, 主要从事无机/高分子复合材料研究. E-mail: zzhang@jlu.edu.cn ;张震东, 男, 博士, 副教授, 主要从事纳米多孔功能材料研究. E-mail: zzddoc@jlu.edu.cn
基金资助:
国家自然科学基金(批准号: 21771081, 21390394, 20971052)、长白山学者奖励计划(批准号: 2014004)和吉林省科技发展计划(批准号: 20180101001JC)资助.

Preparation of Amphiphilic Ti/ZSM-5 Zeolite and Its Catalytic Performance in Oxidative Desulfurization^†

WANG Ying², SUN Chuanyin¹, WANG Runwei¹, ZHANG Zhendong¹(), ZHANG Daming², ZHANG Zongtao¹(), QIU Shilun¹

1. College of Chemistry, State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, Changchun 130012, China
2. College of Electronic Science and Engineering, State Key Laboratory on Integrated Optoelectronics, Jilin University, Changchun 130012, China

Received:2018-11-15 Online:2019-06-10 Published:2019-04-04
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.21771081, 21390394, 20971052), the Changbai Mountain Scholars Program, China(No.2014004) and the Scientific and Technological Development Program of Jilin Province, China(No.20180101001JC).

摘要/Abstract

摘要：

通过使用二苯基硅烷和氨丙基三乙氧基硅烷对Ti/ZSM-5分子筛进行非对称修饰, 获得了外侧亲油、内侧亲水的双亲型催化剂材料am-Ti/ZSM-5. 修饰过程及后处理过程并未破坏分子筛的骨架结构. 样品在不添加萃取剂的情况下, 在以H₂O₂为氧化剂的二苯并噻吩(DBT)氧化脱硫(ODS)反应中表现出高催化活性, 在35 min内可以实现模拟油中DBT的完全脱除. 实验结果表明, 分子筛催化剂的双亲型结构使其在极性-非极性混合体系中具有优异的催化性能.

关键词: 双亲型催化剂, Ti/ZSM-5, 二苯并噻吩, 氧化脱硫

Abstract:

Amphiphilic Ti/ZSM-5 zeolite(am-Ti/ZSM-5) was successfully prepared by asymmetric modification of Ti/ZSM-5 zeolite with diphenylsilane and aminopropyltriethoxysilane. The modification and post-treatment process did not destroy the framework structure of zeolite. The sample showed high catalytic activity in the oxidative desulfurization(ODS) of dibenzothiophene(DBT) using H₂O₂ as the oxidant and without adding the extractant. The complete removal of DBT from the simulated oil can be achieved within 35 min. These results indicate that the unique amphiphilic structure of am-Ti/ZSM-5 makes it have excellent catalytic performance in polar-nonpolar mixtures.

Key words: Amphiphilic catalyst, Ti/ZSM-5, Dibenzothiophene, Oxidative desulfurization

中图分类号:

0643

TrendMD:

王影, 孙传胤, 王润伟, 张震东, 张大明, 张宗弢, 裘式纶. 双亲型Ti/ZSM-5分子筛催化剂的制备及氧化脱硫性能. 高等学校化学学报, 2019, 40(6): 1265.

WANG Ying, SUN Chuanyin, WANG Runwei, ZHANG Zhendong, ZHANG Daming, ZHANG Zongtao, QIU Shilun. Preparation of Amphiphilic Ti/ZSM-5 Zeolite and Its Catalytic Performance in Oxidative Desulfurization^†. Chem. J. Chinese Universities, 2019, 40(6): 1265.

图/表 9

Scheme 1 Synthetic process for amphiphilic zeolite

Fig.1 XRD patterns of am-Ti/ZSM-5-n(A) and various catalysts(B)

Fig.2 UV-Vis spectra of ZSM-5 and am-Ti/ZSM-5-n

Fig.3 Images of contact angle of Ti/ZSM-5-3.0(A, B) and am-Ti/ZSM-5-3.0(C, D)

Fig.4 SEM images of ZSM-5(A), Ti/ZSM-5-3.0(B) and am-Ti/ZSM-5-3.0(C)

Fig.5 TEM images of Ti/ZSM-5-3.0(A) and am-Ti/ZSM-5-3.0(B)

Fig.6 Catalytic performance of am-Ti/ZSM-5-n zeolites with various Ti-content

Fig.7 Desulfurization performance of Ti/ZSM-5-3.0(a) and am-Ti/ZSM-5-3.0(b)

Fig.8 Schematic illustration of ODS of DBT in the presence of am-Ti/ZSM-5

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双亲型Ti/ZSM-5分子筛催化剂的制备及氧化脱硫性能

Preparation of Amphiphilic Ti/ZSM-5 Zeolite and Its Catalytic Performance in Oxidative Desulfurization^†

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双亲型Ti/ZSM-5分子筛催化剂的制备及氧化脱硫性能

Preparation of Amphiphilic Ti/ZSM-5 Zeolite and Its Catalytic Performance in Oxidative Desulfurization†

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Preparation of Amphiphilic Ti/ZSM-5 Zeolite and Its Catalytic Performance in Oxidative Desulfurization^†