Real-time direct transmission electron microscopy imaging of phase and morphology transformation from solid indium oxide hydroxide to hollow corundum-type indium oxide nanocrystallites
Abstract
A time-resolved series of high-resolution transmission electron microscopy (HRTEM) images are used to monitor phase and morphology transformation of rod-like and spherical particles with the initial orthorhombic InOOH phase in situ under continuous illumination with high-energy electrons in a transmission electron microscope. For both particle types, the electron-beam irradiation induces a fast InOOH to rh-In2O3 decomposition accompanied by the formation of voids within the particle/rod center. After illumination time intervals of about 1–2 min (i.e. electron dose 6.3–12.6 × 107 e nm-2) for particles and 8 min (4.3 × 108 e nm-2) for rods, respectively, several small empty cavities become visible in the particle/rod center. The cavities coalesce and form a large hollow space/canal after further illumination. Time-resolved in situ HRTEM unambiguously shows that the formation of internal voids in both nanoparticle types is a consequence of the structural InOOH-to-rh-In2O3 phase transition that starts at the surface of the corresponding particle. The as-formed oxide phase encapsulates the untransformed hydroxylated phase. Its decomposition does not follow the Kirkendall mechanism; the matter transferred outwards is removed in the form of water, leading to void formation inside without an increase of the particle size.
- Authors:
-
[1];
[1];
[3];
[1]
- Fachgebiet Keramische Werkstoffe/Chair of Advanced Ceramic Materials, Institut für Werkstoffwissenschaften und -technologien, Technische Universität Berlin, D-10623 Berlin, Germany
- Laboratorium für Elektronenmikroskopie, Karlsruher Institut für Technologie (KIT), D-76131 Karlsruhe, Germany
- Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, USA
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division (SC-22.3)
- OSTI Identifier:
- 1526651
- Alternate Identifier(s):
- OSTI ID: 1656519
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Nanoscale
- Additional Journal Information:
- Journal Name: Nanoscale Journal Volume: 11 Journal Issue: 25; Journal ID: ISSN 2040-3364
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY
Citation Formats
Schlicker, Lukas, Popescu, Radian, Bekheet, Maged F., Doran, Andrew, Gerthsen, Dagmar, and Gurlo, Aleksander. Real-time direct transmission electron microscopy imaging of phase and morphology transformation from solid indium oxide hydroxide to hollow corundum-type indium oxide nanocrystallites. United Kingdom: N. p., 2019.
Web. doi:10.1039/C9NR02115A.
Schlicker, Lukas, Popescu, Radian, Bekheet, Maged F., Doran, Andrew, Gerthsen, Dagmar, & Gurlo, Aleksander. Real-time direct transmission electron microscopy imaging of phase and morphology transformation from solid indium oxide hydroxide to hollow corundum-type indium oxide nanocrystallites. United Kingdom. https://doi.org/10.1039/C9NR02115A
Schlicker, Lukas, Popescu, Radian, Bekheet, Maged F., Doran, Andrew, Gerthsen, Dagmar, and Gurlo, Aleksander. Thu .
"Real-time direct transmission electron microscopy imaging of phase and morphology transformation from solid indium oxide hydroxide to hollow corundum-type indium oxide nanocrystallites". United Kingdom. https://doi.org/10.1039/C9NR02115A.
@article{osti_1526651,
title = {Real-time direct transmission electron microscopy imaging of phase and morphology transformation from solid indium oxide hydroxide to hollow corundum-type indium oxide nanocrystallites},
author = {Schlicker, Lukas and Popescu, Radian and Bekheet, Maged F. and Doran, Andrew and Gerthsen, Dagmar and Gurlo, Aleksander},
abstractNote = {A time-resolved series of high-resolution transmission electron microscopy (HRTEM) images are used to monitor phase and morphology transformation of rod-like and spherical particles with the initial orthorhombic InOOH phase in situ under continuous illumination with high-energy electrons in a transmission electron microscope. For both particle types, the electron-beam irradiation induces a fast InOOH to rh-In2O3 decomposition accompanied by the formation of voids within the particle/rod center. After illumination time intervals of about 1–2 min (i.e. electron dose 6.3–12.6 × 107 e nm-2) for particles and 8 min (4.3 × 108 e nm-2) for rods, respectively, several small empty cavities become visible in the particle/rod center. The cavities coalesce and form a large hollow space/canal after further illumination. Time-resolved in situ HRTEM unambiguously shows that the formation of internal voids in both nanoparticle types is a consequence of the structural InOOH-to-rh-In2O3 phase transition that starts at the surface of the corresponding particle. The as-formed oxide phase encapsulates the untransformed hydroxylated phase. Its decomposition does not follow the Kirkendall mechanism; the matter transferred outwards is removed in the form of water, leading to void formation inside without an increase of the particle size.},
doi = {10.1039/C9NR02115A},
journal = {Nanoscale},
number = 25,
volume = 11,
place = {United Kingdom},
year = {Thu Jun 27 00:00:00 EDT 2019},
month = {Thu Jun 27 00:00:00 EDT 2019}
}
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https://doi.org/10.1039/C9NR02115A
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Works referenced in this record:
Ag Nanoparticle-Sensitized WO 3 Hollow Nanosphere for Localized Surface Plasmon Enhanced Gas Sensors
journal, July 2016
- Yao, Yao; Ji, Fangxu; Yin, Mingli
- ACS Applied Materials & Interfaces, Vol. 8, Issue 28
An analytical approximation for a size-broadened profile given by the lognormal and gamma distributions
journal, May 2002
- Popa, N. C.; Balzar, D.
- Journal of Applied Crystallography, Vol. 35, Issue 3
C rare earth oxide-corundum transition and crystal chemistry of oxides having the corundum structure
journal, September 1969
- Prewitt, Charles T.; Shannon, Robert D.; Rogers, Donald Burl
- Inorganic Chemistry, Vol. 8, Issue 9
Single-particle mapping of nonequilibrium nanocrystal transformations
journal, November 2016
- Ye, Xingchen; Jones, Matthew R.; Frechette, Layne B.
- Science, Vol. 354, Issue 6314
Electron microscopic study of dehydration transformations. Part III: High resolution observation of the reaction process FeOOH → Fe2O3
journal, June 1983
- Watari, Fumio; Delavignette, P.; Van Landuty, J.
- Journal of Solid State Chemistry, Vol. 48, Issue 1
Quantitative 3D evolution of colloidal nanoparticle oxidation in solution
journal, April 2017
- Sun, Yugang; Zuo, Xiaobing; Sankaranarayanan, Subramanian K. R. S.
- Science, Vol. 356, Issue 6335
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976
- Shannon, R. D.
- Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767
Electron microscopic study of dehydration transformations. I. Twin formation and mosaic structure in hematite derived from goethite
journal, July 1979
- Watari, Fumio; Van Landuyt, J.; Delavignette, P.
- Journal of Solid State Chemistry, Vol. 29, Issue 1
Development of an amorphous mesoporous TiO2 nanosphere as a novel carrier for poorly water-soluble drugs: Effect of different crystal forms of TiO2 carriers on drug loading and release behaviors
journal, May 2012
- Jiang, Haitao; Wang, Tianyi; Wang, Lihong
- Microporous and Mesoporous Materials, Vol. 153
Synthesis, Properties, and Applications of Hollow Micro-/Nanostructures
journal, May 2016
- Wang, Xiaojing; Feng, Ji; Bai, Yaocai
- Chemical Reviews, Vol. 116, Issue 18
Hollow Micro-/Nanostructures: Synthesis and Applications
journal, November 2008
- Lou, Xiong Wen (David); Archer, Lynden A.; Yang, Zichao
- Advanced Materials, Vol. 20, Issue 21
Neutron and X-Ray Crystallographic Studies on Indium Oxide Hydroxide.
journal, January 1970
- Lehmann, M. S.; Larsen, F. Krebs; Poulsen, F. Reibke
- Acta Chemica Scandinavica, Vol. 24
High-spatial-resolution mapping of catalytic reactions on single particles
journal, January 2017
- Wu, Chung-Yeh; Wolf, William J.; Levartovsky, Yehonatan
- Nature, Vol. 541, Issue 7638
A Mesoporous Silica Nanosphere-Based Carrier System with Chemically Removable CdS Nanoparticle Caps for Stimuli-Responsive Controlled Release of Neurotransmitters and Drug Molecules
journal, April 2003
- Lai, Cheng-Yu; Trewyn, Brian G.; Jeftinija, Dusan M.
- Journal of the American Chemical Society, Vol. 125, Issue 15
Compact low power infrared tube furnace for in situ X-ray powder diffraction
journal, January 2017
- Doran, A.; Schlicker, L.; Beavers, C. M.
- Review of Scientific Instruments, Vol. 88, Issue 1
Indium hydroxide to oxide decomposition observed in one nanocrystal during in situ transmission electron microscopy studies
journal, February 2013
- Miehe, Gerhard; Lauterbach, Stefan; Kleebe, Hans-Joachim
- Journal of Solid State Chemistry, Vol. 198
Electron-beam-induced transition aluminas from aluminum trihydroxide
journal, November 2008
- Kim, Y. -M.; Lee, S.; Kim, Y. -S.
- Scripta Materialia, Vol. 59, Issue 9
Electron microscopic study of dehydration transformations. II. The formation of “superstructures” on the dehydration of goethite and diaspore
journal, September 1979
- Watari, Fumio; Delavignette, P.; Amelinckx, S.
- Journal of Solid State Chemistry, Vol. 29, Issue 3
Quantitatively in Situ Imaging Silver Nanowire Hollowing Kinetics
journal, September 2016
- Yu, Le; Yan, Zhongying; Cai, Zhonghou
- Nano Letters, Vol. 16, Issue 10
Scaled-up solvothermal synthesis of nanosized metastable indium oxyhydroxide (InOOH) and corundum-type rhombohedral indium oxide (rh-In2O3)
journal, January 2017
- Schlicker, Lukas; Bekheet, Maged F.; Gurlo, Aleksander
- Zeitschrift für Kristallographie - Crystalline Materials, Vol. 232, Issue 1-3
Hollow nanoparticles as emerging electrocatalysts for renewable energy conversion reactions
journal, January 2018
- Park, Jongsik; Kwon, Taehyun; Kim, Jun
- Chemical Society Reviews, Vol. 47, Issue 22
The kinetics and reaction mechanism of the goethite to hematite transformation
journal, September 1987
- Goss, C. J.
- Mineralogical Magazine, Vol. 51, Issue 361
Nanoengineering of Inorganic and Hybrid Hollow Spheres by Colloidal Templating
journal, November 1998
- Caruso, F.
- Science, Vol. 282, Issue 5391
Dehydration of goethite to hematite from molecular dynamics simulation
journal, June 2010
- Zhang, Wen-Juan; Huo, Chun-Fang; Feng, Gang
- Journal of Molecular Structure: THEOCHEM, Vol. 950, Issue 1-3
Electron Beam-Induced "Nanocalcination" of Boehmite Nanostrips to Mesoporous ?-Alumina Phase
journal, October 2007
- Arami, Hamed; Mazloumi, Mahyar; Khalifehzadeh, Razieh
- Journal of the American Ceramic Society, Vol. 90, Issue 10