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The selective deposition of Fe species inside ZSM-5 for the oxidation of cyclohexane to cyclohexanone

Journal 2021 · IF 9.445 · 64(7): 1088-1095 · 发表于 2021 年 3 月 8 日
作者: Zhai Liming,Zhang Bin,Liang Haojie,Wu Huibin,Yang Xinchun,Luo Gen,Zhao Shichao,Qin Yong
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摘要

The design of efficient iron-based catalysts remains a great challenge for selective cyclohexane oxidation to cyclohexanone under mild conditions. Because of the complex distribution of iron location on the support, the selectivity is always low. Here, we report a general strategy to selectively deposit highly-dispersed FeO x into the micropore of ZSM-5 by atomic layer deposition (ALD). The framework of ZSM-5 and the Brønsted acid sites are intact during ALD, and the Fe species are selectively deposited onto the defect and Lewis acid sites of ZSM-5. Besides, more Fe-O-Si bonds are formed over FeO x /ZSM-5 with a low loading of Fe, while FeO x nanoparticles are generated at high Fe loading. They cannot be realized by the traditional solution method. The obtained FeO x /ZSM-5 catalysts perform high selectivity of cyclohexanone (92%–97%), and ALD cycle numbers of FeO x control the activity. Compared with the Fe nanoparticles, the Fe-O-Si species performs higher turnover frequency and stability in the oxidation reaction.