Facet-specific oxidation of Mn(II) and heterogeneous growth of manganese (oxyhydr)oxides on hematite nanoparticles

Liu, Jing; Inoué, Sayako; Zhu, Runliang; He, Hongping; Hochella, Michael F.

doi:10.1016/j.gca.2021.05.043

Title: Facet-specific oxidation of Mn(II) and heterogeneous growth of manganese (oxyhydr)oxides on hematite nanoparticles

Journal Article · Thu May 27 00:00:00 EDT 2021 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2021.05.043· OSTI ID:1812531

Liu, Jing ^[1];

^[2]; Zhu, Runliang ^[1]; He, Hongping ^[1];

^[3]

Chinese Academy of Sciences (CAS), Guangdong (China). Guangzhou Institute of Geochemistry, CAS Key Laboratory of Mineralogy and Metallogeny/Guangdong Provincial Key Laboratory of Mineral Physics and Materials; Chinese Academy of Sciences (CAS), Beijing (China)
Univ. of Tokyo (Japan). Dept. of Earth and Planetary Science
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Earth and Environment Directorate; Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Geosciences

It is recognized that different facets of minerals vary distinctively in their chemical reactivity with aqueous solutions. However, detailed molecular and atomistic understandings of these phenomena are relatively limited. This study investigated the interaction of aqueous Mn2+ and dissolved oxygen on various facets of two morphology-types of iron oxide (hematite) nanocrystals. These interactions result in the oxidation of manganese and the heterogeneous nucleation and growth of Mn(II)/Mn(III), and Mn(III) oxides. The nanoscale morphology and atomic structure of the manganese oxide products were characterized in detail. Our results, for the first time, directly demonstrate the facet-dependent oxidation of Mn²⁺ and nucleation of Mn(II/III) oxides, followed by their epitaxial growth on hematite. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), and electron diffraction measurements reveal the growth of MnOx nanowires on {012} facets of both hematite nanoplates (HNP) and hematite nanocubes (HNC), while the basal {001} facets on the HNP particles do not produce precipitates. The average oxidation state of the MnO_x on HNP and HNC determined using electron energy-loss spectroscopy (EELS) show that both Mn(II) and Mn(III) are present. The facet-dependent oxidation of Mn²⁺ may be attributed to adsorption-induced electron transfer (ET), and hematite {001} facets generally exhibiting weaker ability in the uptake of ions relative to {012} facets, and the bulk ET from {012} to {001} facets through the conduction band of hematite. Nevertheless, the mineral composition and growth mechanisms of MnOx catalyzed by HNP and HNC are similar. High-resolution TEM analysis reveals the presence of both hausmannite and manganite on HNP and HNC. The nanoscale observations and thermodynamic considerations indicate that the growth mechanisms/processes of MnO_x include heterogeneous nucleation of hausmannite nanoparticles, crystallization by particle attachment, transformation from hausmannite to manganite, and self-catalyzed MnO_x growth. It is possible that all of these processes are concurrent. The crystallographic relationship between the heterogeneously formed manganite with hematite, which has not been reported before, proves that hematite provides reaction sites and functions as an atomic template for the formation of MnO_x nanowires. These findings advance our understanding of the redox chemistry and heterogeneous growth of minerals as controlled by the surficial structure of the substrate mineral. This has important geochemical implications as the catalytic growth of less common, highly reactive phases like MnO_x are known to be consequential in complex natural and anthropogenic environments.

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Research Organization:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; National Natural Science Foundation of China (NSFC); China Postdoctoral Foundation

Grant/Contract Number:: AC05-76RL01830; 41872044; 41902040; 2019M663132

OSTI ID:: 1812531

Report Number(s):: PNNL-SA-158672

Journal Information:: Geochimica et Cosmochimica Acta, Vol. 307; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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