Extraframework Fe-Al-O species occluded in MFI zeolite as the active species in the oxidation of benzene to phenol with nitrous oxide

Extraframework Fe-Al-O species occluded in MFI zeolite as the active species in the oxidation of benzene to phenol with nitrous oxide
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DOI:
10.1016/j.jcat.2003.09.001
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发表时间:
2003-12
影响因子:
7.3
通讯作者:
Ejm Emiel Hensen;Q. Zhu;V. Santen
Ejm Emiel Hensen;Q. Zhu;V. Santen
中科院分区:
化学1区
文献类型:
--
作者:
Ejm Emiel Hensen;Q. Zhu;V. Santen

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MFI 型沸石中苯通过一氧化二氮氧化成苯酚的活性位点的形成需要铁和铝。我们认为活性物质是框架外FeAlO物质。这些物种在暴露于 NO 后产生约 1625 和 1635 cm−1 的特征红外光谱带,这与 Fe 取代的silicalite-1 和 HZSM-5 中发现的特征光谱带不同。虽然我们仅观察到后面这些材料的苯氧化活性可以忽略不计,但含有 Fe 和 Al 的 MFI 沸石表现出良好的性能。此外,我们发现铝合成后分散到铁取代的silicalite-1 中提供了活性材料的替代制备途径。
Iron and aluminum are required for the formation of active sites in MFI-type zeolites for benzene oxidation to phenol by nitrous oxide. We propose that the active species are extraframework FeAlO species. These species produce characteristic IR bands around 1625 and 1635 cm−1after exposure to NO which are different from those found in Fe-substituted silicalite-1 and HZSM-5. While we only observe negligible benzene oxidation activities for these latter materials, a MFI zeolite containing Fe and Al shows good performance. Additionally, we found that postsynthesis dispersion of aluminum to Fe-substituted silicalite-1 offers an alternative preparation route to an active material.