Modification of pillared MFI zeolite nanosheets by nitridation with tailored activity in benzylation of mesitylene and benzyl alcohol

doi:10.1016/j.cjche.2019.03.027

中国化学工程学报 ›› 2019, Vol. 27 ›› Issue (8): 1981-1987.DOI: 10.1016/j.cjche.2019.03.027

• Materials and Product Engineering • 上一篇下一篇

Modification of pillared MFI zeolite nanosheets by nitridation with tailored activity in benzylation of mesitylene and benzyl alcohol

Zhipeng Chen¹, Jiajin Huang¹, Qiaowen Mu¹, Huiyong Chen², Feng Xu³, Yanxiong Fang¹, Baoyu Liu¹

1 School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China;
2 School of Chemical Engineering, Northwest University, Xi'an 710069, China;
3 School of Environment and Chemical Engineering, Foshan University, Foshan 528000, China

收稿日期:2018-07-05 修回日期:2019-02-16 出版日期:2019-08-28 发布日期:2019-11-16
通讯作者: Baoyu Liu
基金资助:
Supported by the Science and Technology Program of Guangzhou, China (201804010172), National Natural Science Foundation of China (21808040, 21706031, 21276052, 21776049), Science and Technology Planning Project of Guangdong Province, China (2012A090300006).

Modification of pillared MFI zeolite nanosheets by nitridation with tailored activity in benzylation of mesitylene and benzyl alcohol

Zhipeng Chen¹, Jiajin Huang¹, Qiaowen Mu¹, Huiyong Chen², Feng Xu³, Yanxiong Fang¹, Baoyu Liu¹

1 School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China;
2 School of Chemical Engineering, Northwest University, Xi'an 710069, China;
3 School of Environment and Chemical Engineering, Foshan University, Foshan 528000, China

Received:2018-07-05 Revised:2019-02-16 Online:2019-08-28 Published:2019-11-16
Contact: Baoyu Liu
Supported by:
Supported by the Science and Technology Program of Guangzhou, China (201804010172), National Natural Science Foundation of China (21808040, 21706031, 21276052, 21776049), Science and Technology Planning Project of Guangdong Province, China (2012A090300006).

摘要/Abstract

摘要： The modification of pillared MFI zeolites was performed by nitridation of silica pillared MFI zeolite nanosheets under NH₃ atmosphere with different time. The resultant zeolites were characterized by a complementary combination of X-ray power diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), pyridine-IR spectroscopy and N₂ adsorption-desorption isotherms. The analyses showed that the nitridation didn't destroy the crystallinity and specific surface area of zeolites, and the acidity of zeolites can be tailored by tuning the time of nitridation, resulting in the different concentration ratios of Brønsted-to-Lewis (B/L) acid sites. Moreover, the nitrided zeolites exhibited high selectivity to 2-benzyl-1,3,5-trimethylbenzene than parent silica pillared MFI zeolite nanosheets in benzylation of mesitylene with benzyl alcohol. A balance between Brønsted acid sites and Lewis acid sites can inhibit the self-etherification of benzyl alcohol and enhance the selectivity of alkylated product. These experimental data implied that nitridation was an effective method to modulate the acidity of zeolites and the synergy between Brønsted acid sites and Lewis acid sites was a decisive factor to determine the selectivity.

关键词: MFI zeolite, Pillar, Nitridation, Benzylation

Abstract: The modification of pillared MFI zeolites was performed by nitridation of silica pillared MFI zeolite nanosheets under NH₃ atmosphere with different time. The resultant zeolites were characterized by a complementary combination of X-ray power diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), pyridine-IR spectroscopy and N₂ adsorption-desorption isotherms. The analyses showed that the nitridation didn't destroy the crystallinity and specific surface area of zeolites, and the acidity of zeolites can be tailored by tuning the time of nitridation, resulting in the different concentration ratios of Brønsted-to-Lewis (B/L) acid sites. Moreover, the nitrided zeolites exhibited high selectivity to 2-benzyl-1,3,5-trimethylbenzene than parent silica pillared MFI zeolite nanosheets in benzylation of mesitylene with benzyl alcohol. A balance between Brønsted acid sites and Lewis acid sites can inhibit the self-etherification of benzyl alcohol and enhance the selectivity of alkylated product. These experimental data implied that nitridation was an effective method to modulate the acidity of zeolites and the synergy between Brønsted acid sites and Lewis acid sites was a decisive factor to determine the selectivity.

Key words: MFI zeolite, Pillar, Nitridation, Benzylation

Zhipeng Chen, Jiajin Huang, Qiaowen Mu, Huiyong Chen, Feng Xu, Yanxiong Fang, Baoyu Liu. Modification of pillared MFI zeolite nanosheets by nitridation with tailored activity in benzylation of mesitylene and benzyl alcohol[J]. 中国化学工程学报, 2019, 27(8): 1981-1987.

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Modification of pillared MFI zeolite nanosheets by nitridation with tailored activity in benzylation of mesitylene and benzyl alcohol

Modification of pillared MFI zeolite nanosheets by nitridation with tailored activity in benzylation of mesitylene and benzyl alcohol

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