Trimodal Porous Hierarchical SSZ-13 Zeolite with Improved Catalytic Performance in the Methanol-to-Olefins Reaction

被引：126

作者：

Zhu, Xiaochun ^{[1
]}

Hofmann, Jan P. ^{[1
]}

Mezari, Brahim ^{[1
]}

Kosinov, Nikolay ^{[1
]}

Wu, Leilei ^{[1
]}

Qian, Qingyun ^{[2
]}

Weckhuysen, Bert M. ^{[2
]}

Asahina, Shunsuke ^{[3
]}

Ruiz-Martinez, Javier ^{[2
]}

Hensen, Emiel J. M. ^{[1
]}

机构：

[1] Eindhoven Univ Technol, Dept Chem Engn & Chem, Inorgan Mat Chem, Schuit Inst Catalysis, POB 513, NL-5600 MB Eindhoven, Netherlands

[2] Univ Utrecht, Debye Inst Nanomat Sci, Inorgan Chem & Catalysis, Univ 99, NL-3584 CG Utrecht, Netherlands

[3] JEOL Ltd, Akishima, Tokyo 1968558, Japan

来源：

ACS CATALYSIS | 2016年 / 6卷 / 04期

关键词：

zeolite; SSZ-13; porosity; deactivation; carbonaceous deposits; methanol-to-olefins; SOLID-STATE NMR; H-1 MAS NMR; SILICA CHA ZEOLITES; MOLECULAR-SIEVES; CO-REACTION; ALL-SILICA; UV/VIS MICROSPECTROSCOPY; HYDROCARBON FORMATION; CHABAZITE H-SSZ-13; REACTION-MECHANISM;

D O I：

10.1021/acscatal.5b02480

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Chabazite zeolites with trimodal porosity (native micropores of the CHA framework, an additional network of larger micropores of similar to 0.5 nm, and mesopores) were synthesized by adding diquarternary ammonium type surfactant C22-4-4 cations and fluoride anions in the synthesis of SSZ-13 zeolite. The hierarchical SSZ-13 zeolites are fully crystalline and exhibit similar acidity as bulk SSZ-13 zeolite. The increased diffusion rate in the hierarchical SSZ-13, proven by uptake experiments of bulky molecules and selective staining by thiophene oligomers, resulted in much slower catalyst deactivation in the methanol-to-olefins (MTO) reaction. Confocal fluorescent images of spent hierarchical SSZ-13 zeolites reveal homogeneous distribution of carbonaceous deposits, indicating that the micropore space has been completely utilized during the MTO reaction.

引用

页码：2163 / 2177

页数：15

共 67 条

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