Rapid Diffusion and Nanosegregation of Hydrogen in Magnesium Alloys from Exposure to Water
Abstract
Hydrogen gas is formed when Mg corrodes in water; however, the manner and extent to which the hydrogen may also enter the Mg metal is poorly understood. Such knowledge is critical as stress corrosion cracking (SCC)/embrittlement phenomena limit many otherwise promising structural and functional uses of Mg. Here, we report via D2O/D isotopic tracer and H2O exposures with characterization by secondary ion mass spectrometry, inelastic neutron scattering vibrational spectrometry, electron microscopy, and atom probe tomography techniques direct evidence that hydrogen rapidly penetrated tens of micrometers into Mg metal after only 4 h of exposure to water at room temperature. Further, technologically important microalloying additions of <1 wt % Zr and Nd used to improve the manufacturability and mechanical properties of Mg significantly increased the extent of hydrogen ingress, whereas Al additions in the 2–3 wt % range did not. Segregation of hydrogen species was observed at regions of high Mg/Zr/Nd nanoprecipitate density and at Mg(Zr) metastable solid solution microstructural features. We also report evidence that this ingressed hydrogen was unexpectedly present in the alloy as nanoconfined, molecular H2. These new insights provide a basis for strategies to design Mg alloys to resist SCC in aqueous environments as well as potentiallymore »
- Authors:
-
- Oak Ridge National Laboratory (ORNL), Oak Ridge, Tennessee 37831, United States
- Department of Geological Sciences, University of Manitoba (UM), Winnipeg, MB R3T 2N2, Canada
- Magnesium Elektron North America (MENA), Madison, Illinois 62060, United States
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
- OSTI Identifier:
- 1400005
- Alternate Identifier(s):
- OSTI ID: 1408592
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Published Article
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Name: ACS Applied Materials and Interfaces Journal Volume: 9 Journal Issue: 43; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 08 HYDROGEN; 36 MATERIALS SCIENCE; corrosion; hydrogen; hydrogen storage; magnesium; stress corrosion cracking (SCC)
Citation Formats
Brady, Michael P., Ievlev, Anton V., Fayek, Mostafa, Leonard, Donovan N., Frith, Matthew G., Meyer, III, Harry M., Ramirez-Cuesta, Anibal J., Daemen, Luke L., Cheng, Yongqiang, Guo, Wei, Poplawsky, Jonathan D., Ovchinnikova, Olga S., Thomson, Jeffrey, Anovitz, Lawrence M., Rother, Gernot, Shin, Dongwon, Song, Guang-Ling, and Davis, Bruce. Rapid Diffusion and Nanosegregation of Hydrogen in Magnesium Alloys from Exposure to Water. United States: N. p., 2017.
Web. doi:10.1021/acsami.7b10750.
Brady, Michael P., Ievlev, Anton V., Fayek, Mostafa, Leonard, Donovan N., Frith, Matthew G., Meyer, III, Harry M., Ramirez-Cuesta, Anibal J., Daemen, Luke L., Cheng, Yongqiang, Guo, Wei, Poplawsky, Jonathan D., Ovchinnikova, Olga S., Thomson, Jeffrey, Anovitz, Lawrence M., Rother, Gernot, Shin, Dongwon, Song, Guang-Ling, & Davis, Bruce. Rapid Diffusion and Nanosegregation of Hydrogen in Magnesium Alloys from Exposure to Water. United States. https://doi.org/10.1021/acsami.7b10750
Brady, Michael P., Ievlev, Anton V., Fayek, Mostafa, Leonard, Donovan N., Frith, Matthew G., Meyer, III, Harry M., Ramirez-Cuesta, Anibal J., Daemen, Luke L., Cheng, Yongqiang, Guo, Wei, Poplawsky, Jonathan D., Ovchinnikova, Olga S., Thomson, Jeffrey, Anovitz, Lawrence M., Rother, Gernot, Shin, Dongwon, Song, Guang-Ling, and Davis, Bruce. Wed .
"Rapid Diffusion and Nanosegregation of Hydrogen in Magnesium Alloys from Exposure to Water". United States. https://doi.org/10.1021/acsami.7b10750.
@article{osti_1400005,
title = {Rapid Diffusion and Nanosegregation of Hydrogen in Magnesium Alloys from Exposure to Water},
author = {Brady, Michael P. and Ievlev, Anton V. and Fayek, Mostafa and Leonard, Donovan N. and Frith, Matthew G. and Meyer, III, Harry M. and Ramirez-Cuesta, Anibal J. and Daemen, Luke L. and Cheng, Yongqiang and Guo, Wei and Poplawsky, Jonathan D. and Ovchinnikova, Olga S. and Thomson, Jeffrey and Anovitz, Lawrence M. and Rother, Gernot and Shin, Dongwon and Song, Guang-Ling and Davis, Bruce},
abstractNote = {Hydrogen gas is formed when Mg corrodes in water; however, the manner and extent to which the hydrogen may also enter the Mg metal is poorly understood. Such knowledge is critical as stress corrosion cracking (SCC)/embrittlement phenomena limit many otherwise promising structural and functional uses of Mg. Here, we report via D2O/D isotopic tracer and H2O exposures with characterization by secondary ion mass spectrometry, inelastic neutron scattering vibrational spectrometry, electron microscopy, and atom probe tomography techniques direct evidence that hydrogen rapidly penetrated tens of micrometers into Mg metal after only 4 h of exposure to water at room temperature. Further, technologically important microalloying additions of <1 wt % Zr and Nd used to improve the manufacturability and mechanical properties of Mg significantly increased the extent of hydrogen ingress, whereas Al additions in the 2–3 wt % range did not. Segregation of hydrogen species was observed at regions of high Mg/Zr/Nd nanoprecipitate density and at Mg(Zr) metastable solid solution microstructural features. We also report evidence that this ingressed hydrogen was unexpectedly present in the alloy as nanoconfined, molecular H2. These new insights provide a basis for strategies to design Mg alloys to resist SCC in aqueous environments as well as potentially impact functional uses such as hydrogen storage where increased hydrogen uptake is desired.},
doi = {10.1021/acsami.7b10750},
journal = {ACS Applied Materials and Interfaces},
number = 43,
volume = 9,
place = {United States},
year = {2017},
month = {10}
}
https://doi.org/10.1021/acsami.7b10750
Web of Science
Works referenced in this record:
Metal hydride materials for solid hydrogen storage: A review☆
journal, June 2007
- Sakintuna, B.; Lamaridarkrim, F.; Hirscher, M.
- International Journal of Hydrogen Energy, Vol. 32, Issue 9
Enhanced Corrosion Resistance and Biocompatibility of Magnesium Alloy by Mg–Al-Layered Double Hydroxide
journal, December 2016
- Peng, Feng; Li, Hua; Wang, Donghui
- ACS Applied Materials & Interfaces, Vol. 8, Issue 51
A Study on Factors Affecting the Degradation of Magnesium and a Magnesium-Yttrium Alloy for Biomedical Applications
journal, June 2013
- Johnson, Ian; Liu, Huinan
- PLoS ONE, Vol. 8, Issue 6
A thermodynamic database for zirconium alloys
journal, November 1999
- Dupin, N.; Ansara, I.; Servant, C.
- Journal of Nuclear Materials, Vol. 275, Issue 3
New nanostructured phases with reversible hydrogen storage capability in immiscible magnesium–zirconium system produced by high-pressure torsion
journal, April 2016
- Edalati, Kaveh; Emami, Hoda; Ikeda, Yuji
- Acta Materialia, Vol. 108
Stress Corrosion Cracking and Hydrogen Diffusion in Magnesium
journal, August 2006
- Atrens, A.; Winzer, N.; Song, G.
- Advanced Engineering Materials, Vol. 8, Issue 8
Hydrogen-induced decomposition of Zr-rich cores in an Mg−6Zn−0.6Zr−0.5Cu alloy
journal, September 2012
- Sha, G.; Zhu, H. M.; Liu, J. W.
- Acta Materialia, Vol. 60, Issue 15
Insights from a Recent Meeting: Current Status and Future Directions in Magnesium Corrosion Research
journal, May 2017
- Brady, Michael P.; Joost, William J.; David Warren, C.
- CORROSION, Vol. 73, Issue 5
Role of hydrogen in deformed magnesium alloys of the Mg-Zn-Zr-REM system
journal, March 2008
- Volkova, E. F.; Morozova, G. I.
- Metal Science and Heat Treatment, Vol. 50, Issue 3-4
Rechargeable magnesium battery: Current status and key challenges for the future
journal, October 2014
- Saha, Partha; Datta, Moni Kanchan; Velikokhatnyi, Oleg I.
- Progress in Materials Science, Vol. 66
Corrosion of Zirconium Alloys Used for Nuclear Fuel Cladding
journal, July 2015
- Motta, Arthur T.; Couet, Adrien; Comstock, Robert J.
- Annual Review of Materials Research, Vol. 45, Issue 1
Corrosion mechanism and hydrogen evolution on Mg
journal, April 2015
- Thomas, S.; Medhekar, N. V.; Frankel, G. S.
- Current Opinion in Solid State and Materials Science, Vol. 19, Issue 2
Effects of Hydrogen on the Mechanical Properties of Pure Magnesium
journal, January 2011
- Chino, Yasumasa; Nishihara, Daiki; Ueda, Takamichi
- MATERIALS TRANSACTIONS, Vol. 52, Issue 6
Fundamentals and advances in magnesium alloy corrosion
journal, August 2017
- Esmaily, M.; Svensson, J. E.; Fajardo, S.
- Progress in Materials Science, Vol. 89
General and Localized Corrosion of Magnesium Alloys: A Critical Review
journal, February 2004
- Ghali, Edward; Dietzel, Wolfgang; Kainer, Karl-Ulrich
- Journal of Materials Engineering and Performance, Vol. 13, Issue 1
First Principles Modeling of Cathodic Reaction Thermodynamics in Dilute Magnesium Alloys
journal, May 2017
- Limmer, Krista R.; Williams, Kristen S.; Labukas, Joseph P.
- CORROSION, Vol. 73, Issue 5
On the early stages of precipitation in dilute Mg–Nd alloys
journal, April 2016
- Natarajan, Anirudh Raju; Solomon, Ellen L. S.; Puchala, Brian
- Acta Materialia, Vol. 108
The Effect of Absorbed Hydrogen on the Corrosion of Steels: Review, Discussion, and Implications
journal, April 2017
- Thomas, S.; Sundararajan, G.; White, P. D.
- CORROSION, Vol. 73, Issue 4
Hydrogen Embrittlement of Magnesium and Magnesium Alloys: A Review
journal, January 2013
- Kappes, Mariano; Iannuzzi, Mariano; Carranza, Ricardo M.
- Journal of The Electrochemical Society, Vol. 160, Issue 4
A First-Principles Surface Reaction Kinetic Model for Hydrogen Evolution under Cathodic and Anodic Conditions on Magnesium
journal, January 2016
- Taylor, Christopher D.
- Journal of The Electrochemical Society, Vol. 163, Issue 9
Atom probe tomography observation of hydrogen in high-Mn steel and silver charged via an electrolytic route
journal, August 2014
- Haley, D.; Merzlikin, S. V.; Choi, P.
- International Journal of Hydrogen Energy, Vol. 39, Issue 23
The texture and anisotropy of magnesium–zinc–rare earth alloy sheets
journal, April 2007
- Bohlen, Jan; Nürnberg, Marcus R.; Senn, Jeremy W.
- Acta Materialia, Vol. 55, Issue 6
In situ site-specific specimen preparation for atom probe tomography
journal, February 2007
- Thompson, K.; Lawrence, D.; Larson, D. J.
- Ultramicroscopy, Vol. 107, Issue 2-3
Transmission Electron Microscopy Study of Aqueous Film Formation and Evolution on Magnesium Alloys
journal, January 2014
- Unocic, K. A.; Elsentriecy, H. H.; Brady, Michael P.
- Journal of The Electrochemical Society, Vol. 161, Issue 6
A Critical Review of the Stress Corrosion Cracking (SCC) of Magnesium Alloys
journal, August 2005
- Winzer, N.; Atrens, A.; Song, G.
- Advanced Engineering Materials, Vol. 7, Issue 8
Review of Recent Developments in the Field of Magnesium Corrosion: Recent Developments in Mg Corrosion
journal, January 2015
- Atrens, Andrej; Song, Guang-Ling; Liu, Ming
- Advanced Engineering Materials, Vol. 17, Issue 4
Tracer Film Growth Study of Hydrogen and Oxygen from the Corrosion of Magnesium in Water
journal, January 2014
- Brady, M. P.; Fayek, M.; Elsentriecy, H. H.
- Journal of The Electrochemical Society, Vol. 161, Issue 9
Corrosion of magnesium alloys: the role of alloying
journal, October 2014
- Gusieva, K.; Davies, C. H. J.; Scully, J. R.
- International Materials Reviews, Vol. 60, Issue 3
Quantum rattling of molecular hydrogen in clathrate hydrate nanocavities
journal, October 2007
- Ulivi, L.; Celli, M.; Giannasi, A.
- Physical Review B, Vol. 76, Issue 16
Effect of Hydrogen on Corrosion and Stress Corrosion Cracking of AZ91 Alloy in Aqueous Solutions
journal, January 2016
- Chen, Jian; Wang, Jian-Qiu; Han, En-Hou
- Acta Metallurgica Sinica (English Letters), Vol. 29, Issue 1
Introductory lecture on corrosion chemistry: a focus on anodic hydrogen evolution on Al and Mg
journal, January 2015
- Frankel, G. S.; Fajardo, S.; Lynch, B. M.
- Faraday Discussions, Vol. 180
Film Breakdown and Nano-Porous Mg(OH) 2 Formation from Corrosion of Magnesium Alloys in Salt Solutions
journal, January 2015
- Brady, M. P.; Rother, G.; Anovitz, L. M.
- Journal of The Electrochemical Society, Vol. 162, Issue 4