Direct synthesis of propylene glycol methyl ether from propylene using an Al-TS-1 catalyst: Ti-Al synergy

被引:1
|
作者
Guo, Yanke [1 ,2 ]
Qin, Qiaoyun [1 ,2 ]
Zhu, Jing [1 ,2 ]
Wang, Baohe [1 ,2 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn, 90 Weijin Rd, Tianjin 300072, Peoples R China
[2] Tianjin Univ, R&D Ctr Petrochem Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, Peoples R China
基金
中国国家自然科学基金;
关键词
POWDER NEUTRON-DIFFRACTION; NMR CHEMICAL-SHIFTS; MFI FRAMEWORK; TS-1; TITANIUM; OXIDE; PERFORMANCE; MECHANISMS; TRANSITION; NONRANDOM;
D O I
10.1039/d3nj00194f
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Propylene glycol methyl ether was directly synthesized from propylene and hydrogen peroxide under mild conditions via aluminum modified titanium silicalite-1 as a bifunctional catalyst. It has both active sites capable of epoxidation and active sites capable of ring opening reactions, thus realizing the one-pot preparation of propylene glycol methyl ether by propylene. The synergistic effect of Ti-Al on the catalytic performance and the distribution of propylene glycol methyl ether isomer were investigated in detail, and the synergistic catalysis between the two active sites was characterized. The gradual introduction of aluminum reduced the activation ability for hydrogen peroxide, but gradually increased the selectivity for propylene glycol methyl ether. Under the optimum conditions, the selectivity for propylene glycol methyl ether reached 91.53%. Combined with Density Functional Theory (DFT) calculations, the synergistic catalytic effect of doped Al and framework Ti in titanium silicalite-1 is discussed in detail from a microscopic perspective. Al increases the Lewis acid strength of Ti active sites and promotes the conversion of propylene to propylene oxide (PO), and simultaneously Ti increases the Bronsted acid strength of Al active sites and promotes the conversion of propylene oxide to propylene glycol ether.
引用
收藏
页码:7810 / 7818
页数:9
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