4.6 Article

Catalytically active species in bifunctional Aluminum-Containing titanium Silicalite-1 zeolite for ethylene epoxidation

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CHEMICAL ENGINEERING SCIENCE
卷 282, 期 -, 页码 -

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PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ces.2023.119241

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Aluminum-containing titanium silicalite-1; Ethylene epoxidation; Catalytic active species; UV resonance Raman spectroscopy; Nuclear magnetic resonance spectroscopy

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In this study, post-treated Al-TS-1 catalysts were prepared through hydrothermal post-treatments, which showed higher H2O2 conversion in the HPEG process compared to the parent Al-TS-1. The post-treatment also affected the location and amount of framework Al species in the catalyst, but had minor impact on the EG selectivity.
Aluminum-containing titanium silicalite-1 zeolite (Al-TS-1) is an important bifunctional catalyst for green production of ethylene glycol (EG) via a hydrogen peroxide/ethylene process (HPEG). In this work, hydrothermal post-treatments are carried out to a parent Al-TS-1 in (NH4)(2)CO3 aqueous solutions under varied conditions to produce post-treated Al-TS-1 catalysts. In addition to the framework Ti(OSi)(4) species found in both the parent and post-treated Al-TS-1 catalysts, the post-treated catalysts also contain Ti(OH)(4)(OSi)(2) species. For HPEG process, the post-treated Al-TS-1 delivers a significantly higher H2O2 conversion than the parent Al-TS-1. This is attributed to the outstanding catalytic activity of Ti(OH)(4)(OSi)(2) which is similar to 16.8 times the activity of Ti(OSi)(4). Furthermore, although the parent and post-treated Al-TS-1 contain both the framework and extra-framework Al species, the post-treatment is also found to alter the detailed location and amount of framework Al species in the catalyst. Such changes, however, have only minor effect on the EG selectivity.

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