Evaluation of Mg Compounds as Coating Materials in Mg Batteries
Abstract
Mg batteries utilizing a Mg metal anode with a high-voltage intercalation cathode define a potential pathway toward energy storage with high energy density. However, the making of Mg batteries is plagued by the instability of existing electrolytes against the Mg-metal anode and high-voltage cathode materials. One viable solution to this problem is the identification of protective coating materials that could effectively separate the distinct chemistries of the metal-anode and the cathode materials from the electrolyte. Using first-principles calculations we mapped the electrochemical stability windows for non-redox-active Mg binary and ternary compounds in order to identify potential coating materials for Mg batteries. Our results identify Mg-halides and Mg(BH4)2 as promising anode coating materials based on their significant reductive stability. On the cathode side, we single out MgF2, Mg(PO3)2, and MgP4O11 as effective passivating agents.
- Authors:
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1492876
- Alternate Identifier(s):
- OSTI ID: 1560589
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Frontiers in Chemistry
- Additional Journal Information:
- Journal Name: Frontiers in Chemistry Journal Volume: 7; Journal ID: ISSN 2296-2646
- Publisher:
- Frontiers Research Foundation
- Country of Publication:
- Switzerland
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 36 MATERIALS SCIENCE; Mg batteries; first-principles calculation; density functional theory; coating materials; intercalation batteries; solid electrolytes; multivalent ion batteries
Citation Formats
Chen, Tina, Ceder, Gerbrand, Sai Gautam, Gopalakrishnan, and Canepa, Pieremanuele. Evaluation of Mg Compounds as Coating Materials in Mg Batteries. Switzerland: N. p., 2019.
Web. doi:10.3389/fchem.2019.00024.
Chen, Tina, Ceder, Gerbrand, Sai Gautam, Gopalakrishnan, & Canepa, Pieremanuele. Evaluation of Mg Compounds as Coating Materials in Mg Batteries. Switzerland. https://doi.org/10.3389/fchem.2019.00024
Chen, Tina, Ceder, Gerbrand, Sai Gautam, Gopalakrishnan, and Canepa, Pieremanuele. Wed .
"Evaluation of Mg Compounds as Coating Materials in Mg Batteries". Switzerland. https://doi.org/10.3389/fchem.2019.00024.
@article{osti_1492876,
title = {Evaluation of Mg Compounds as Coating Materials in Mg Batteries},
author = {Chen, Tina and Ceder, Gerbrand and Sai Gautam, Gopalakrishnan and Canepa, Pieremanuele},
abstractNote = {Mg batteries utilizing a Mg metal anode with a high-voltage intercalation cathode define a potential pathway toward energy storage with high energy density. However, the making of Mg batteries is plagued by the instability of existing electrolytes against the Mg-metal anode and high-voltage cathode materials. One viable solution to this problem is the identification of protective coating materials that could effectively separate the distinct chemistries of the metal-anode and the cathode materials from the electrolyte. Using first-principles calculations we mapped the electrochemical stability windows for non-redox-active Mg binary and ternary compounds in order to identify potential coating materials for Mg batteries. Our results identify Mg-halides and Mg(BH4)2 as promising anode coating materials based on their significant reductive stability. On the cathode side, we single out MgF2, Mg(PO3)2, and MgP4O11 as effective passivating agents.},
doi = {10.3389/fchem.2019.00024},
journal = {Frontiers in Chemistry},
number = ,
volume = 7,
place = {Switzerland},
year = {Wed Jan 30 00:00:00 EST 2019},
month = {Wed Jan 30 00:00:00 EST 2019}
}
Free Publicly Available Full Text
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https://doi.org/10.3389/fchem.2019.00024
https://doi.org/10.3389/fchem.2019.00024
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Cited by: 43 works
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Figures / Tables:
FIGURE 1: Periodic table highlighting the non-transition-metal elements that form binary (and ternary) compounds with Mg (red), including triels (Group IIIA, green), tetrels (Group IVA, light blue), pnictogens (Group VA, yellow), chalcogens (Group VIA, gray), halogens (Group VIIA, orange), and other elements (Hydrogen, purple). We considered all Mg-X binaries andmore »
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Works referenced in this record:
Understanding the Initial Stages of Reversible Mg Deposition and Stripping in Inorganic Nonaqueous Electrolytes
journal, April 2015
- Canepa, Pieremanuele; Gautam, Gopalakrishnan Sai; Malik, Rahul
- Chemistry of Materials, Vol. 27, Issue 9
Role of Point Defects in Spinel Mg Chalcogenide Conductors
journal, November 2017
- Canepa, Pieremanuele; Sai Gautam, Gopalakrishnan; Broberg, Danny
- Chemistry of Materials, Vol. 29, Issue 22
Challenges for Rechargeable Li Batteries
journal, February 2010
- Goodenough, John B.; Kim, Youngsik
- Chemistry of Materials, Vol. 22, Issue 3, p. 587-603
Generating derivative structures at a fixed concentration
journal, June 2012
- Hart, Gus L. W.; Nelson, Lance J.; Forcade, Rodney W.
- Computational Materials Science, Vol. 59
How General is the Conversion Reaction in Mg Battery Cathode: A Case Study of the Magnesiation of α-MnO 2
journal, August 2015
- Ling, Chen; Zhang, Ruigang; Arthur, Timothy S.
- Chemistry of Materials, Vol. 27, Issue 16
Odyssey of Multivalent Cathode Materials: Open Questions and Future Challenges
journal, February 2017
- Canepa, Pieremanuele; Sai Gautam, Gopalakrishnan; Hannah, Daniel C.
- Chemical Reviews, Vol. 117, Issue 5
A high capacity thiospinel cathode for Mg batteries
journal, January 2016
- Sun, Xiaoqi; Bonnick, Patrick; Duffort, Victor
- Energy & Environmental Science, Vol. 9, Issue 7
Spinel compounds as multivalent battery cathodes: a systematic evaluation based on ab initio calculations
journal, January 2015
- Liu, Miao; Rong, Ziqin; Malik, Rahul
- Energy & Environmental Science, Vol. 8, Issue 3
High magnesium mobility in ternary spinel chalcogenides
journal, November 2017
- Canepa, Pieremanuele; Bo, Shou-Hang; Sai Gautam, Gopalakrishnan
- Nature Communications, Vol. 8, Issue 1
On the Way to Rechargeable Mg Batteries: The Challenge of New Cathode Materials †
journal, February 2010
- Levi, E.; Gofer, Y.; Aurbach, D.
- Chemistry of Materials, Vol. 22, Issue 3
Structural Analysis of Electrolyte Solutions for Rechargeable Mg Batteries by Stereoscopic Means and DFT Calculations
journal, April 2011
- Pour, Nir; Gofer, Yossi; Major, Dan T.
- Journal of the American Chemical Society, Vol. 133, Issue 16
Influence of Inversion on Mg Mobility and Electrochemistry in Spinels
journal, September 2017
- Sai Gautam, Gopalakrishnan; Canepa, Pieremanuele; Urban, Alexander
- Chemistry of Materials, Vol. 29, Issue 18
Design of electrolyte solutions for Li and Li-ion batteries: a review
journal, November 2004
- Aurbach, Doron; Talyosef, Yosef; Markovsky, Boris
- Electrochimica Acta, Vol. 50, Issue 2-3
Algorithm for generating derivative structures
journal, June 2008
- Hart, Gus L. W.; Forcade, Rodney W.
- Physical Review B, Vol. 77, Issue 22
A lithium superionic conductor
journal, July 2011
- Kamaya, Noriaki; Homma, Kenji; Yamakawa, Yuichiro
- Nature Materials, Vol. 10, Issue 9, p. 682-686
Coordination Chemistry in magnesium battery electrolytes: how ligands affect their performance
journal, November 2013
- Shao, Yuyan; Liu, Tianbiao; Li, Guosheng
- Scientific Reports, Vol. 3, Issue 1
Structural Analysis of Magnesium Chloride Complexes in Dimethoxyethane Solutions in the Context of Mg Batteries Research
journal, November 2017
- Salama, Michael; Shterenberg, Ivgeni; J. W. Shimon, Linda
- The Journal of Physical Chemistry C, Vol. 121, Issue 45
Micromorphological Studies of Lithium Electrodes in Alkyl Carbonate Solutions Using in Situ Atomic Force Microscopy
journal, December 2000
- Cohen, Yaron S.; Cohen, Yair; Aurbach, Doron
- The Journal of Physical Chemistry B, Vol. 104, Issue 51
Prototype systems for rechargeable magnesium batteries
journal, October 2000
- Aurbach, D.; Lu, Z.; Schechter, A.
- Nature, Vol. 407, Issue 6805, p. 724-727
The Nature of the Chemical Bond. iv. the Energy of Single Bonds and the Relative Electronegativity of Atoms
journal, September 1932
- Pauling, Linus
- Journal of the American Chemical Society, Vol. 54, Issue 9
High-power all-solid-state batteries using sulfide superionic conductors
journal, March 2016
- Kato, Yuki; Hori, Satoshi; Saito, Toshiya
- Nature Energy, Vol. 1, Issue 4
Mg rechargeable batteries: an on-going challenge
journal, January 2013
- Yoo, Hyun Deog; Shterenberg, Ivgeni; Gofer, Yosef
- Energy & Environmental Science, Vol. 6, Issue 8, p. 2265-2279
Improved electrolytes for Li-ion batteries: Mixtures of ionic liquid and organic electrolyte with enhanced safety and electrochemical performance
journal, February 2010
- Guerfi, A.; Dontigny, M.; Charest, P.
- Journal of Power Sources, Vol. 195, Issue 3
Novel, electrolyte solutions comprising fully inorganic salts with high anodic stability for rechargeable magnesium batteries
journal, January 2014
- Doe, Robert E.; Han, Ruoban; Hwang, Jaehee
- Chemical Communications, Vol. 50, Issue 2, p. 243-245
On the electrochemical behavior of magnesium electrodes in polar aprotic electrolyte solutions
journal, May 1999
- Lu, Z.; Schechter, A.; Moshkovich, M.
- Journal of Electroanalytical Chemistry, Vol. 466, Issue 2, p. 203-217
First-Principles Study of the Voltage Profile and Mobility of Mg Intercalation in a Chromium Oxide Spinel
journal, December 2017
- Chen, Tina; Sai Gautam, Gopalakrishnan; Huang, Wenxuan
- Chemistry of Materials, Vol. 30, Issue 1
A review of advanced and practical lithium battery materials
journal, January 2011
- Marom, Rotem; Amalraj, S. Francis; Leifer, Nicole
- Journal of Materials Chemistry, Vol. 21, Issue 27
Electrodeposited Bi, Sb and Bi1-xSbx alloys as anodes for Mg-ion batteries
journal, March 2012
- Arthur, Timothy S.; Singh, Nikhilendra; Matsui, Masaki
- Electrochemistry Communications, Vol. 16, Issue 1
XPS Investigation of Surface Chemistry of Magnesium Electrodes in Contact with Organic Solutions of Organochloroaluminate Complex Salts
journal, March 2003
- Gofer, Yossi; Turgeman, Rachel; Cohen, H.
- Langmuir, Vol. 19, Issue 6
Inhomogeneous Electron Gas
journal, March 1973
- Rajagopal, A. K.; Callaway, J.
- Physical Review B, Vol. 7, Issue 5
Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965
- Kohn, W.; Sham, L. J.
- Physical Review, Vol. 140, Issue 4A, p. A1133-A1138
A review of the features and analyses of the solid electrolyte interphase in Li-ion batteries
journal, September 2010
- Verma, Pallavi; Maire, Pascal; Novák, Petr
- Electrochimica Acta, Vol. 55, Issue 22, p. 6332-6341
Magnesium Borohydride: From Hydrogen Storage to Magnesium Battery
journal, August 2012
- Mohtadi, Rana; Matsui, Masaki; Arthur, Timothy S.
- Angewandte Chemie International Edition, Vol. 51, Issue 39, p. 9780-9783
Effect of Concentration on the Electrochemistry and Speciation of the Magnesium Aluminum Chloride Complex Electrolyte Solution
journal, October 2017
- See, Kimberly A.; Liu, Yao-Min; Ha, Yeyoung
- ACS Applied Materials & Interfaces, Vol. 9, Issue 41
Electrolyte Solutions for Rechargeable Magnesium Batteries Based on Organomagnesium Chloroaluminate Complexes
journal, January 2002
- Aurbach, Doron; Gizbar, Haim; Schechter, Alex
- Journal of The Electrochemical Society, Vol. 149, Issue 2, p. A115-A121
Elucidating the structure of the magnesium aluminum chloride complex electrolyte for magnesium-ion batteries
journal, January 2015
- Canepa, Pieremanuele; Jayaraman, Saivenkataraman; Cheng, Lei
- Energy & Environmental Science, Vol. 8, Issue 12
On the Balance of Intercalation and Conversion Reactions in Battery Cathodes
journal, April 2018
- Hannah, Daniel C.; Sai Gautam, Gopalakrishnan; Canepa, Pieremanuele
- Advanced Energy Materials, Vol. 8, Issue 20
Enhanced Stability of the Carba- closo -dodecaborate Anion for High-Voltage Battery Electrolytes through Rational Design
journal, July 2018
- Hahn, Nathan T.; Seguin, Trevor J.; Lau, Ka-Cheong
- Journal of the American Chemical Society, Vol. 140, Issue 35
Interfacial Stability of Li Metal–Solid Electrolyte Elucidated via in Situ Electron Microscopy
journal, October 2016
- Ma, Cheng; Cheng, Yongqiang; Yin, Kuibo
- Nano Letters, Vol. 16, Issue 11
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation
journal, July 2013
- Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy
- APL Materials, Vol. 1, Issue 1
Manganese Dioxide As Rechargeable Magnesium Battery Cathode
journal, November 2017
- Ling, Chen; Zhang, Ruigang
- Frontiers in Energy Research, Vol. 5
Boron Clusters as Highly Stable Magnesium-Battery Electrolytes
journal, February 2014
- Carter, Tyler J.; Mohtadi, Rana; Arthur, Timothy S.
- Angewandte Chemie International Edition, Vol. 53, Issue 12
Lithium ions on the fast track
journal, August 2011
- Masquelier, Christian
- Nature Materials, Vol. 10, Issue 9
The Interplay of Al and Mg Speciation in Advanced Mg Battery Electrolyte Solutions
journal, December 2015
- See, Kimberly A.; Chapman, Karena W.; Zhu, Lingyang
- Journal of the American Chemical Society, Vol. 138, Issue 1
A high-throughput infrastructure for density functional theory calculations
journal, June 2011
- Jain, Anubhav; Hautier, Geoffroy; Moore, Charles J.
- Computational Materials Science, Vol. 50, Issue 8
Study of Electrochemical Phenomena Observed at the Mg Metal/Electrolyte Interface
journal, December 2016
- Tutusaus, Oscar; Mohtadi, Rana; Singh, Nikhilendra
- ACS Energy Letters, Vol. 2, Issue 1
Practical Stability Limits of Magnesium Electrolytes
journal, January 2016
- Lipson, Albert L.; Han, Sang-Don; Pan, Baofei
- Journal of The Electrochemical Society, Vol. 163, Issue 10
Electrical Properties and Cation Migration in MgMn2O4
journal, January 1964
- Rosenberg, M.; Nicolau, P.
- physica status solidi (b), Vol. 6, Issue 1
Quest for Nonaqueous Multivalent Secondary Batteries: Magnesium and Beyond
journal, October 2014
- Muldoon, John; Bucur, Claudiu B.; Gregory, Thomas
- Chemical Reviews, Vol. 114, Issue 23
Interface Stability in Solid-State Batteries
journal, December 2015
- Richards, William D.; Miara, Lincoln J.; Wang, Yan
- Chemistry of Materials, Vol. 28, Issue 1
Interfacial Insight from Operando XAS/TEM for Magnesium Metal Deposition with Borohydride Electrolytes
journal, August 2017
- Arthur, Timothy S.; Glans, Per-Anders; Singh, Nikhilendra
- Chemistry of Materials, Vol. 29, Issue 17
An Efficient Halogen-Free Electrolyte for Use in Rechargeable Magnesium Batteries
journal, May 2015
- Tutusaus, Oscar; Mohtadi, Rana; Arthur, Timothy S.
- Angewandte Chemie, Vol. 127, Issue 27
Generating derivative structures from multilattices: Algorithm and application to hcp alloys
journal, July 2009
- Hart, Gus L. W.; Forcade, Rodney W.
- Physical Review B, Vol. 80, Issue 1
The Intercalation Phase Diagram of Mg in V 2 O 5 from First-Principles
journal, May 2015
- Sai Gautam, Gopalakrishnan; Canepa, Pieremanuele; Abdellahi, Aziz
- Chemistry of Materials, Vol. 27, Issue 10
Electrolyte roadblocks to a magnesium rechargeable battery
journal, January 2012
- Muldoon, John; Bucur, Claudiu B.; Oliver, Allen G.
- Energy & Environmental Science, Vol. 5, Issue 3, p. 5941-5950
Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction
journal, December 2015
- Bachman, John Christopher; Muy, Sokseiha; Grimaud, Alexis
- Chemical Reviews, Vol. 116, Issue 1
Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis
journal, February 2013
- Ong, Shyue Ping; Richards, William Davidson; Jain, Anubhav
- Computational Materials Science, Vol. 68
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