Oxidation induced strain and defects in magnetite crystals

Ke Yuan; Sang Soo Lee; Wonsuk Cha; Andrew Ulvestad; Hyunjung Kim; Bektur Abdilla; Neil C. Sturchio; Paul Fenter

doi:10.1038/s41467-019-08470-0

Oxidation induced strain and defects in magnetite crystals

Ke Yuan, Sang Soo Lee, Wonsuk Cha, Andrew Ulvestad, Hyunjung Kim, Bektur Abdilla, Neil C. Sturchio, Paul Fenter

Research output: Contribution to journal › Article › peer-review

47 Scopus citations

Abstract

Oxidation of magnetite (Fe ₃ O ₄ ) 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. 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.

Original language	English
Article number	703
Journal	Nature Communications
Volume	10
Issue number	1
DOIs	https://doi.org/10.1038/s41467-019-08470-0
State	Published - Dec 1 2019
Externally published	Yes

Funding

This work was supported by U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division under Contract DE-AC02-06CH11357 to UChicago Argonne, LLC, Operator of Argonne National Laboratory (“Argonne”). Argonne, a U.S. Department of Energy Office of Science laboratory. This research used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility, beamline 34-ID-C, operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract no. DE-AC02-06CH11357. The U.S. Government retains for itself, and others acting on its behalf, a paid-up nonexclusive, irrevocable worldwide license in said article to reproduce, prepare derivative works, distribute copies to the public, and perform publicly and display publicly, by or on behalf of the Government. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan. H.K. thanks the support by the National Research Foundation of Korea (NRF-2014R1A2A1A10052454 and 2015R1A5A1009962). Finally, we thank Dr. Brian Stephenson (Argonne National Laboratory) for helpful discussions and Kyuseok Yun (Sogang University) for data visualization.

Funders	Funder number
DOE Office of Science
Office of Basic Energy Sciences
U.S. Department of Energy
Office of Science
Argonne National Laboratory
Chemical Sciences, Geosciences, and Biosciences Division	DE-AC02-06CH11357
National Research Foundation of Korea	2015R1A5A1009962, NRF-2014R1A2A1A10052454

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abstract = " Oxidation of magnetite (Fe 3 O 4 ) 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. 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.",

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Oxidation induced strain and defects in magnetite crystals

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