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Title: Oxidation induced strain and defects in magnetite crystals

Abstract

Oxidation of magnetite (Fe3O4) has broad implications in geochemistry, environmental science and materials science. Spatially resolving strain fields and defect evolution during oxidation of magnetite provides further insight into its reaction mechanisms. Here we show that the morphology and internal strain distributions within individual nano-sized (~400 nm) magnetite crystals can be visualized using Bragg coherent diffractive imaging (BCDI). Oxidative dissolution in acidic solutions leads to increases in the magnitude and heterogeneity of internal strains. This heterogeneous strain likely results from lattice distortion caused by Fe(II) diffusion that leads to the observed domains of increasing compressive and tensile strains. In contrast, strain evolution is less pronounced during magnetite oxidation at elevated temperature in air. Furthermore, these results demonstrate that oxidative dissolution of magnetite can induce a rich array of strain and defect structures, which could be an important factor that contributes to the high reactivity observed on magnetite particles in aqueous environment.

Authors:
 [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [3]; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Sogang Univ., Seoul (Korea)
  3. Univ. of Delaware, Newark, DE (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1494579
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Yuan, Ke, Lee, Sang Soo, Cha, Wonsuk, Ulvestad, Andrew, Kim, Hyunjung, Abdilla, Bektur, Sturchio, Neil C., and Fenter, Paul. Oxidation induced strain and defects in magnetite crystals. United States: N. p., 2019. Web. doi:10.1038/s41467-019-08470-0.
Yuan, Ke, Lee, Sang Soo, Cha, Wonsuk, Ulvestad, Andrew, Kim, Hyunjung, Abdilla, Bektur, Sturchio, Neil C., & Fenter, Paul. Oxidation induced strain and defects in magnetite crystals. United States. https://doi.org/10.1038/s41467-019-08470-0
Yuan, Ke, Lee, Sang Soo, Cha, Wonsuk, Ulvestad, Andrew, Kim, Hyunjung, Abdilla, Bektur, Sturchio, Neil C., and Fenter, Paul. Mon . "Oxidation induced strain and defects in magnetite crystals". United States. https://doi.org/10.1038/s41467-019-08470-0. https://www.osti.gov/servlets/purl/1494579.
@article{osti_1494579,
title = {Oxidation induced strain and defects in magnetite crystals},
author = {Yuan, Ke and Lee, Sang Soo and Cha, Wonsuk and Ulvestad, Andrew and Kim, Hyunjung and Abdilla, Bektur and Sturchio, Neil C. and Fenter, Paul},
abstractNote = {Oxidation of magnetite (Fe3O4) has broad implications in geochemistry, environmental science and materials science. Spatially resolving strain fields and defect evolution during oxidation of magnetite provides further insight into its reaction mechanisms. Here we show that the morphology and internal strain distributions within individual nano-sized (~400 nm) magnetite crystals can be visualized using Bragg coherent diffractive imaging (BCDI). Oxidative dissolution in acidic solutions leads to increases in the magnitude and heterogeneity of internal strains. This heterogeneous strain likely results from lattice distortion caused by Fe(II) diffusion that leads to the observed domains of increasing compressive and tensile strains. In contrast, strain evolution is less pronounced during magnetite oxidation at elevated temperature in air. Furthermore, these results demonstrate that oxidative dissolution of magnetite can induce a rich array of strain and defect structures, which could be an important factor that contributes to the high reactivity observed on magnetite particles in aqueous environment.},
doi = {10.1038/s41467-019-08470-0},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Mon Feb 11 00:00:00 EST 2019},
month = {Mon Feb 11 00:00:00 EST 2019}
}

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Cited by: 31 works
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Figures / Tables:

Fig. 1 Fig. 1: Dissolution of a pyramid-shaped magnetite crystal observed ex situ after reaction in 0.1 M HCl solution for 14 min. a, b were the 3D volume viewed from two different perspectives at a 30% amplitude threshold. The lattice displacements along the [311] direction were projected on the isosurfaces. cmore » 3D strain structure associated with compressive (blue, strain <−0.00035 shown in Fig. 3b) and tensile (red, strain > 0.00035 shown in Fig. 3b) strains. d Cross-sectional views of the internal strain field of the plane indicated by the dashed lines in (a) and (b). Magnetite d311= 2.5314 Å43. Scale bar, 200 nm« less

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Atomic-scale structure and properties of highly stable antiphase boundary defects in Fe3O4
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  • Nature Communications, Vol. 5, Issue 1
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Three-dimensional imaging of strain in a single ZnO nanorod
journal, December 2009

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  • Nature Materials, Vol. 9, Issue 2
  • DOI: 10.1038/nmat2607

Core–shell strain structure of zeolite microcrystals
journal, July 2013

  • Cha, Wonsuk; Jeong, Nak Cheon; Song, Sanghoon
  • Nature Materials, Vol. 12, Issue 8
  • DOI: 10.1038/nmat3698

Three-dimensional imaging of dislocation propagation during crystal growth and dissolution
journal, June 2015

  • Clark, Jesse N.; Ihli, Johannes; Schenk, Anna S.
  • Nature Materials, Vol. 14, Issue 8
  • DOI: 10.1038/nmat4320

The self-healing of defects induced by the hydriding phase transformation in palladium nanoparticles
journal, November 2017


Size dependent microbial oxidation and reduction of magnetite nano- and micro-particles
journal, August 2016

  • Byrne, James M.; van der Laan, Gerrit; Figueroa, Adriana I.
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep30969

Formation energies and relative stability of perfect and faulted dislocation loops in silicon
journal, June 2000

  • Cristiano, F.; Grisolia, J.; Colombeau, B.
  • Journal of Applied Physics, Vol. 87, Issue 12
  • DOI: 10.1063/1.373557

Magnetite morphology and life on Mars
journal, November 2001

  • Buseck, P. R.; Dunin-Borkowski, R. E.; Devouard, B.
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  • DOI: 10.1073/pnas.241387898

One-Dimensional Fast Migration of Vacancy Clusters in Metals
journal, November 2007


Bragg coherent diffractive imaging of single-grain defect dynamics in polycrystalline films
journal, May 2017


The Symmetry of Ordered Cubic γ-Fe2O3 Investigated by TEM
journal, June 2006

  • Kelm, Klemens; Mader, Werner
  • Zeitschrift für Naturforschung B, Vol. 61, Issue 6
  • DOI: 10.1515/znb-2006-0605

Magnetite from magnetotactic bacteria; size distributions and twinning
journal, December 1998

  • Devouard, Bertrand; Posfai, Mihaly; Hua, Xin
  • American Mineralogist, Vol. 83, Issue 11-12 Part 2
  • DOI: 10.2138/am-1998-11-1228

A simple inorganic process for formation of carbonates, magnetite, and sulfides in Martian meteorite ALH84001
journal, March 2001

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  • American Mineralogist, Vol. 86, Issue 3
  • DOI: 10.2138/am-2001-2-321

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.