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Fe Doped MIL-101/Graphene Nanohybrid for Photocatalytic Oxidation of Alcohols Under Visible-Light Irradiation

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Abstract

A novel photoactive porous material of GR/FeMIL-101 based on FeMIL-101 metal organic frameworks (MOFs) was successfully synthesized via a simple hydrothermal method. The structural and photoelectric properties of the GR/FeMIL-101 was analyzed by XRD, SEM, TEM, TGA, XPS, UV–vis DRS, FT-IR, PL and EIS methods. The photocatalytic performance for the selective oxidation of benzyl alcohol with GR/FeMIL-101 as catalysts was evaluated under visible light irradiation. The results showed that the GR/FeMIL-101 nanohybrid had better photocatalytic performance than both of FeMIL-101 and the pristine MIL-101. It was further found that the incorporation of Fe and MIL-101 caused valence fluctuations of Fe3+/Fe2+ which improved the absorption of visible-light and increased the separation efficiency of photogenerated charges. In addition, the combination of FeMIL-101 and GR could further promote the transfer rate of the photoelectrons. The mechanism of the reaction revealed that ·O2− was the dominating active specie in this reaction through active species trapping experiments.

Graphic Abstract

Fe doped MIL-101/GR nanohybrid was successfully synthesized as an efficient photocatalyst for selective oxidation of alcohols under visible-light and shown a best conversion of 50%. Analyses revealed that Fe was successfully doped into the MIL-101, valence fluctuation of Fe2+/Fe3+ not only improved the visible-light absorption but also increased the separation rate of photoexcited carriers. Graphene further improved the transportation rate of electron (e-). Subsequently, the possible photocatalytic mechanism for the selective oxidation of alcohols was proposed. It was proved that superoxide radicals (·O2-) was the main active species when the reaction was performed under Oxygen atmosphere.

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Acknowledgements

The research was financially supported by NSFC (52063026, 21563026), the Program for Changjiang Scholars and Innovative Research Team in University (IRT15R56), the Innovation Team Basic Scientific Research Project of Gansu Province (1606RJIA324), and the Science and Technology Program of Gansu Province (19JR2RA020). We also thank the Key Laboratory of Eco-functional Polymer Materials (Northwest Normal University), Ministry of Education, and the Gansu International Scientific and Technological Cooperation Base of Water-Retention Chemical Functional Materials, for financial support.

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Authors and Affiliations

  1. Key Laboratory of Polymer Materials of Gansu Province, Key Laboratory of Eco-Functional Polymer Materials, Ministry of Education, College of Chemistry and Chemical Engineering, Northwest Normal University, Lanzhou, 730070, China

    Mingming Wang, Yali Ma, Bolin Lv, Fenglin Hua, Shuangyan Meng, Xuedi Lei, Qingtao Wang, Bitao Su, Ziqiang Lei & Zhiwang Yang

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  1. Mingming Wang
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Correspondence to Zhiwang Yang.

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Wang, M., Ma, Y., Lv, B. et al. Fe Doped MIL-101/Graphene Nanohybrid for Photocatalytic Oxidation of Alcohols Under Visible-Light Irradiation. Catal Lett 151, 2384–2395 (2021). https://doi.org/10.1007/s10562-020-03472-w

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