A novel MOFs-induced strategy for preparing anatase-free hierarchical TS-1 zeolite:synthesis routes, growth mechanisms and enhanced catalytic performance

被引:16
作者
An, Guoqing [1 ]
Wang, Chang'an [1 ,4 ]
Gao, Hongyi [1 ,3 ]
Wang, Ge [1 ]
Luo, Yibin [2 ]
Liu, Zhiyuan [1 ]
Xia, Changjiu [2 ]
Liu, Siqi [1 ]
Peng, Xinxin [2 ]
Cheng, Zhixiang [1 ]
Shu, Xingtian [2 ]
机构
[1] Univ Sci & Technol Beijing, Beijing Adv Innovat Ctr Mat Genome Engn, Sch Mat Sci & Engn, Beijing Key Lab Funct Mat Mol & Struct Constructio, Beijing 100083, Peoples R China
[2] SINOPEC, Res Inst Petr Proc, Beijing 100083, Peoples R China
[3] SINOPEC Changling Branch Co, Yueyang 414012, Peoples R China
[4] Univ Sci & Technol Beijing, Shunde Grad Sch, Shunde 528399, Peoples R China
关键词
MOFs-induced; Anatase-free; Hierarchical TS-1; Synthetic strategy; Crystal growth mechanisms; Catalytic performance; TITANIUM SILICALITE-1; PROPYLENE EPOXIDATION; ASSISTED SYNTHESIS; ZEOLITE; HYDROXYLATION; OXIDATION; SURFACE;
D O I
10.1016/j.jcis.2022.10.113
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
Titanosilicate-1 zeolites (TS-1) as one of the most commonly used catalysts for alkene epoxidation, con-struction of hierarchical pores as well as elimination of anatase to promote mass transportation and avoid invalid decomposition of hydrogen peroxide are always desirable yet challenging goals. Here, a novel and unique Ti-based metal organic frameworks (MOFs)-induced synthetic strategy for fabricating anatase-free hierarchical TS-1 was first proposed. All the components of MOFs perform different functions: the uniformly distributed Ti nodes replace conventional tetrabutyl titanate (TBOT) to serve as sole Ti source for constructing zeolite crystal; the separated ligands can be embedded in the zeolite framework and act as template to in situ build hierarchical pore structure; the coordination interaction between Ti nodes and ligands can efficiently avoid the anatase generation by balancing the forming rates of Ti-OH and Si-OH. This synthetic strategy is of general applicability, and two different synthetic routes including tra-ditional hydrothermal process and steam assisted crystallization (SAC) procedure are successfully adopted. The obtained hydrothermal TS-1 and SAC anatase-free samples all possess abundant intercrys-talline mesopores of 20-50 nm and even macropores between 50 and 150 nm, improving the conversion over 25 % for 1 hexene epoxidation than TS-1 sample prepared by conventional route. The influences of the amount of Ti MOFs precursor and the crystallization process are studied in detail, and possible synthesis mechanisms are proposed. This MOFs-induced strategy might open up an avenue for the rational design of ideal and hierarchical zeolite to boost the catalytic efficiency.(c) 2022 Published by Elsevier Inc.
引用
收藏
页码:291 / 302
页数:12
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