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Probing the Structure and Binding Mode of EDTA on the Surface of Mn3O4 Nanoparticles for Water Oxidation by Advanced Electron Paramagnetic Resonance Spectroscopy

Title
Probing the Structure and Binding Mode of EDTA on the Surface of Mn3O4 Nanoparticles for Water Oxidation by Advanced Electron Paramagnetic Resonance Spectroscopy
Authors
Kim, JinPark, SunghakGo, Yoo KyungJin, KyoungsukKim, YujeongNam, Ki TaeKim, Sun Hee
Ewha Authors
김선희
Issue Date
2020
Journal Title
INORGANIC CHEMISTRY
ISSN
0020-1669JCR Link

1520-510XJCR Link
Citation
INORGANIC CHEMISTRY vol. 59, no. 13, pp. 8846 - 8854
Publisher
AMER CHEMICAL SOC
Indexed
SCIE; SCOPUS WOS
Document Type
Article
Abstract
Identification of the surface structure of nanoparticles is important for understanding the catalytic mechanism and improving the properties of the particles. Here, we provide a detailed description of the coordination modes of ethylenediaminetetraacetate (EDTA) on Mn3O4 nanoparticles at the atomic level, as obtained by advanced electron paramagnetic resonance (EPR) spectroscopy. Binding of EDTA to Mn3O4 leads to dramatic changes in the EPR spectrum, with a 5-fold increase in the axial zero-field splitting parameter of Mn(II). This indicates significant changes in the coordination environment of the Mn(II) site; hence, the binding of EDTA causes a profound change in the electronic structure of the manganese site. Furthermore, the electron spin echo envelope modulation results reveal that two N-14 atoms of EDTA are directly coordinated to the Mn site and a water molecule is coordinated to the surface of the nanoparticles. An Fourier transform infrared spectroscopy study shows that the Ca(II) ion is coordinated to the carboxylic ligands via the pseudobridging mode. The EPR spectroscopic results provide an atomic picture of surface-modified Mn3O4 nanoparticles for the first time. These results can enhance our understanding of the rational design of catalysts, for example, for the water oxidation reaction.
DOI
10.1021/acs.inorgchem.0c00611
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자연과학대학 > 화학·나노과학전공 > Journal papers
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