Weakly hydrophobic nanoconfinement by graphene aerogels greatly enhances the reactivity and ambient stability of reactivity of MIL-101-Fe in Fenton-like reaction

Yuwei Zhang; Fei Liu; Zhichao Yang; Jieshu Qian; Bingcai Pan

doi:10.1007/s12274-020-3239-1

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Research Article

Weakly hydrophobic nanoconfinement by graphene aerogels greatly enhances the reactivity and ambient stability of reactivity of MIL-101-Fe in Fenton-like reaction

Yuwei Zhang^¹, Fei Liu^¹, Zhichao Yang^², Jieshu Qian^{¹^,³}(

), Bingcai Pan^{²^,³}

1 Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China

2 State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China

3 Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing 210023, China

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Graphical Abstract

Abstract

In the pursuit of heterogeneous catalysts with high reactivity, metal organic framework (MOF) nanomaterials have received tremendous attentions. However, many MOF catalysts especially Fe-based MOFs need to be utilized immediately after synthesis or being activated using high temperature, because of the easy loss of reactivity in humid environments resulting from the occupation of active Fe sites by water molecules. Here, we describe an inspiring strategy of growing MIL-101-Fe nanoparticles inside the three-dimensional confined space of graphene aerogel (GA), generating shapeable GA/MIL-101-Fe nanocomposite convenient for practical use. Compared to MIL-101-Fe, GA/MIL-101-Fe as catalyst demonstrates much higher reactivity in Fenton-like reaction, attributing to smaller MIL-101-Fe particle size, presence of active Fe(II) sites, and abundant defects in GA. Strikingly, the weakly hydrophobic nature of the composite greatly inhibits the loss of catalytic reactivity after being stored in humid air and accelerates the recovery of reactivity in mild temperature, by resisting the entrance of water molecules and helping to exclude water molecules. This work demonstrates that a delicate design of nanocomposite structure could not only improve the reactivity of the catalytic component, but also overcome its intrinsic drawback by taking advantage of the properties of host. We hope this functional nanoconfinement strategy could be extended to more scenarios in other fields.

Keywords

nanoconfinement hydrophobicity MIL-101-Fe graphene aerogel Fenton-like reaction

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Nano Research

Volume 14 Issue 7,
July 2021

Pages 2383-2389

DOI: 10.1007/s12274-020-3239-1

Cite this article:

Zhang Y, Liu F, Yang Z, et al. Weakly hydrophobic nanoconfinement by graphene aerogels greatly enhances the reactivity and ambient stability of reactivity of MIL-101-Fe in Fenton-like reaction. Nano Research, 2021, 14(7): 2383-2389. https://doi.org/10.1007/s12274-020-3239-1

Topics:

Aerogels Catalysts Graphene Metals Nanocomposites Organic frameworks Organometallics Oxidation Particle size Synthesis (chemical)

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Received: 25 August 2020

Revised: 11 November 2020

Accepted: 13 November 2020

Published: 05 July 2021