Development of Safe and Sustainable Dual-Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes
Abstract
In this study, a new dual-ion battery (DIB) concept based on an aqueous/non-aqueous electrolyte is reported, combining high safety in the form of a nonflammable water-in-salt electrolyte, a high cathodic stability by forming a protective interphase on the negative electrode (non-aqueous solvent), and improved sustainability by using a graphite-based positive electrode material. Far beyond the anodic stability limit of water, the formation of a stage-2 acceptor-type graphite intercalation compound (GIC) of bis(trifluoromethanesulfonyl) imide (TFSI) anions from an aqueous-based electrolyte is achieved for the first time, as confirmed by ex-situ X-ray diffraction. The choice of negative electrode material shows a huge impact on the performance of the DIB cell chemistry, i.e., discharge capacities up to 40 mAh g–1 are achieved even at a high specific current of 200 mA g–1. In particular, lithium titanium phosphate (LiTi2(PO4)3; LTP) and lithium titanium oxide (Li4Ti5O12; LTO) are evaluated as negative electrodes, exhibiting specific advantages for this DIB setup. In this work, a new DIB storage concept combining an environmentally friendly, transition-metal-free, abundant graphite positive electrode material, and a nonflammable water-based electrolyte is established, thus paving the path toward a sustainable and safe alternative energy storage technology.
- Authors:
-
- Univ. of Münster (Germany)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Forschungszentrum Juelich, Münster (Germany)
- Publication Date:
- Research Org.:
- Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program; German Federal Ministry of Education and Research (BMBF); Ministry of Economic Affairs, Innovation, Digitalization and Energy of the State of North Rhine-Westphalia (MWIDE)
- OSTI Identifier:
- 1719113
- Report Number(s):
- PNNL-SA-145659
Journal ID: ISSN 1614-6832
- Grant/Contract Number:
- AC05-76RL01830; 03XP0118; 313-W044A
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 8; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; anion intercalation; aqueous batteries; dual-ion batteries; graphite intercalation compounds; hybrid aqueous/nonaqueous electrolytes
Citation Formats
Wrogemann, Jens Matthies, Künne, Sven, Heckmann, Andreas, Rodríguez‐Pérez, Ismael A., Siozios, Vassilios, Yan, Bo, Li, Jie, Winter, Martin, Beltrop, Kolja, and Placke, Tobias. Development of Safe and Sustainable Dual-Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes. United States: N. p., 2020.
Web. doi:10.1002/aenm.201902709.
Wrogemann, Jens Matthies, Künne, Sven, Heckmann, Andreas, Rodríguez‐Pérez, Ismael A., Siozios, Vassilios, Yan, Bo, Li, Jie, Winter, Martin, Beltrop, Kolja, & Placke, Tobias. Development of Safe and Sustainable Dual-Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes. United States. https://doi.org/10.1002/aenm.201902709
Wrogemann, Jens Matthies, Künne, Sven, Heckmann, Andreas, Rodríguez‐Pérez, Ismael A., Siozios, Vassilios, Yan, Bo, Li, Jie, Winter, Martin, Beltrop, Kolja, and Placke, Tobias. Wed .
"Development of Safe and Sustainable Dual-Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes". United States. https://doi.org/10.1002/aenm.201902709. https://www.osti.gov/servlets/purl/1719113.
@article{osti_1719113,
title = {Development of Safe and Sustainable Dual-Ion Batteries Through Hybrid Aqueous/Nonaqueous Electrolytes},
author = {Wrogemann, Jens Matthies and Künne, Sven and Heckmann, Andreas and Rodríguez‐Pérez, Ismael A. and Siozios, Vassilios and Yan, Bo and Li, Jie and Winter, Martin and Beltrop, Kolja and Placke, Tobias},
abstractNote = {In this study, a new dual-ion battery (DIB) concept based on an aqueous/non-aqueous electrolyte is reported, combining high safety in the form of a nonflammable water-in-salt electrolyte, a high cathodic stability by forming a protective interphase on the negative electrode (non-aqueous solvent), and improved sustainability by using a graphite-based positive electrode material. Far beyond the anodic stability limit of water, the formation of a stage-2 acceptor-type graphite intercalation compound (GIC) of bis(trifluoromethanesulfonyl) imide (TFSI) anions from an aqueous-based electrolyte is achieved for the first time, as confirmed by ex-situ X-ray diffraction. The choice of negative electrode material shows a huge impact on the performance of the DIB cell chemistry, i.e., discharge capacities up to 40 mAh g–1 are achieved even at a high specific current of 200 mA g–1. In particular, lithium titanium phosphate (LiTi2(PO4)3; LTP) and lithium titanium oxide (Li4Ti5O12; LTO) are evaluated as negative electrodes, exhibiting specific advantages for this DIB setup. In this work, a new DIB storage concept combining an environmentally friendly, transition-metal-free, abundant graphite positive electrode material, and a nonflammable water-based electrolyte is established, thus paving the path toward a sustainable and safe alternative energy storage technology.},
doi = {10.1002/aenm.201902709},
journal = {Advanced Energy Materials},
number = 8,
volume = 10,
place = {United States},
year = {Wed Jan 15 00:00:00 EST 2020},
month = {Wed Jan 15 00:00:00 EST 2020}
}
Works referenced in this record:
Performance and cost of materials for lithium-based rechargeable automotive batteries
journal, April 2018
- Schmuch, Richard; Wagner, Ralf; Hörpel, Gerhard
- Nature Energy, Vol. 3, Issue 4
Rechargeable Dual‐Ion Batteries with Graphite as a Cathode: Key Challenges and Opportunities
journal, August 2019
- Kravchyk, Kostiantyn V.; Kovalenko, Maksym V.
- Advanced Energy Materials, Vol. 9, Issue 35
Expanding the Cathodic Potential Window of Activated Carbon Electrodes in a Lithium-Salt Containing Electrolyte
journal, October 2018
- Dsoke, Sonia
- Batteries & Supercaps, Vol. 1, Issue 6
Aqueous Li-ion battery enabled by halogen conversion–intercalation chemistry in graphite
journal, May 2019
- Yang, Chongyin; Chen, Ji; Ji, Xiao
- Nature, Vol. 569, Issue 7755
Hydrate-melt electrolytes for high-energy-density aqueous batteries
journal, August 2016
- Yamada, Yuki; Usui, Kenji; Sodeyama, Keitaro
- Nature Energy, Vol. 1, Issue 10
An Aqueous Dual‐Ion Battery Cathode of Mn 3 O 4 via Reversible Insertion of Nitrate
journal, April 2019
- Jiang, Heng; Wei, Zhixuan; Ma, Lu
- Angewandte Chemie International Edition, Vol. 58, Issue 16
The Development and Future of Lithium Ion Batteries
journal, December 2016
- Blomgren, George E.
- Journal of The Electrochemical Society, Vol. 164, Issue 1
Does Size really Matter? New Insights into the Intercalation Behavior of Anions into a Graphite-Based Positive Electrode for Dual-Ion Batteries
journal, August 2016
- Beltrop, Kolja; Meister, Paul; Klein, Sven
- Electrochimica Acta, Vol. 209
4.0 V Aqueous Li-Ion Batteries
journal, September 2017
- Yang, Chongyin; Chen, Ji; Qing, Tingting
- Joule, Vol. 1, Issue 1
Über Graphitsalze
journal, June 1938
- Rüdorff, W.; Hofmann, U.
- Zeitschrift für anorganische und allgemeine Chemie, Vol. 238, Issue 1
Perspective on Performance, Cost, and Technical Challenges for Practical Dual-Ion Batteries
journal, December 2018
- Placke, Tobias; Heckmann, Andreas; Schmuch, Richard
- Joule, Vol. 2, Issue 12
Advanced aqueous rechargeable lithium battery using nanoparticulate LiTi2(PO4)3/C as a superior anode
journal, June 2015
- Sun, Dan; Jiang, Yifan; Wang, Haiyan
- Scientific Reports, Vol. 5, Issue 1
Intercalation compounds of graphite
journal, January 2002
- Dresselhaus, M. S.; Dresselhaus, G.
- Advances in Physics, Vol. 51, Issue 1
Lithium ion, lithium metal, and alternative rechargeable battery technologies: the odyssey for high energy density
journal, May 2017
- Placke, Tobias; Kloepsch, Richard; Dühnen, Simon
- Journal of Solid State Electrochemistry, Vol. 21, Issue 7
Towards high-performance dual-graphite batteries using highly concentrated organic electrolytes
journal, January 2018
- Heckmann, Andreas; Thienenkamp, Johannes; Beltrop, Kolja
- Electrochimica Acta, Vol. 260
Fluorine-free water-in-ionomer electrolytes for sustainable lithium-ion batteries
journal, December 2018
- He, Xin; Yan, Bo; Zhang, Xin
- Nature Communications, Vol. 9, Issue 1
Electrochemical intercalation of bis(fluorosulfonyl)amide anions into graphite from aqueous solutions
journal, March 2019
- Kondo, Yasuyuki; Miyahara, Yuto; Fukutsuka, Tomokazu
- Electrochemistry Communications, Vol. 100
Energy and Capacity Projections for Practical Dual-Graphite Cells
journal, January 2000
- Dahn, J. R.; Seel, J. A.
- Journal of The Electrochemical Society, Vol. 147, Issue 3
X-ray diffraction studies of the electrochemical intercalation of bis(trifluoromethanesulfonyl)imide anions into graphite for dual-ion cells
journal, October 2013
- Schmuelling, Guido; Placke, Tobias; Kloepsch, Richard
- Journal of Power Sources, Vol. 239
Dual-ion Cells Based on Anion Intercalation into Graphite from Ionic Liquid-Based Electrolytes
journal, June 2012
- Placke, Tobias; Bieker, Peter; Lux, Simon Franz
- Zeitschrift für Physikalische Chemie, Vol. 226, Issue 5-6
Advanced High-Voltage Aqueous Lithium-Ion Battery Enabled by “Water-in-Bisalt” Electrolyte
journal, April 2016
- Suo, Liumin; Borodin, Oleg; Sun, Wei
- Angewandte Chemie International Edition, Vol. 55, Issue 25
Alternative electrochemical energy storage: potassium-based dual-graphite batteries
journal, January 2017
- Beltrop, K.; Beuker, S.; Heckmann, A.
- Energy & Environmental Science, Vol. 10, Issue 10
The Solid Electrolyte Interphase – The Most Important and the Least Understood Solid Electrolyte in Rechargeable Li Batteries
journal, December 2009
- Winter, Martin
- Zeitschrift für Physikalische Chemie, Vol. 223, Issue 10-11
Recent Progress in Graphite Intercalation Compounds for Rechargeable Metal (Li, Na, K, Al)-Ion Batteries
journal, June 2017
- Xu, Jiantie; Dou, Yuhai; Wei, Zengxi
- Advanced Science, Vol. 4, Issue 10
Reversible Intercalation of Bis(trifluoromethanesulfonyl)imide Anions from an Ionic Liquid Electrolyte into Graphite for High Performance Dual-Ion Cells
journal, January 2012
- Placke, Tobias; Fromm, Olga; Lux, Simon Franz
- Journal of The Electrochemical Society, Vol. 159, Issue 11
Influence of Graphite Characteristics on the Electrochemical Intercalation of Bis(trifluoromethanesulfonyl) imide Anions into a Graphite-Based Cathode
journal, January 2013
- Placke, Tobias; Rothermel, Sergej; Fromm, Olga
- Journal of The Electrochemical Society, Vol. 160, Issue 11
Electrochemical properties of TiP2O7 and LiTi2(PO4)3 as anode material for lithium ion battery with aqueous solution electrolyte
journal, February 2007
- Wang, Haibo; Huang, Kelong; Zeng, Yuqun
- Electrochimica Acta, Vol. 52, Issue 9
Unravelling charge/discharge and capacity fading mechanisms in dual-graphite battery cells using an electron inventory model
journal, September 2019
- Heidrich, Bastian; Heckmann, Andreas; Beltrop, Kolja
- Energy Storage Materials, Vol. 21
"Water-in-salt" electrolyte enables high-voltage aqueous lithium-ion chemistries
journal, November 2015
- Suo, L.; Borodin, O.; Gao, T.
- Science, Vol. 350, Issue 6263
Hybrid Aqueous/Non-aqueous Electrolyte for Safe and High-Energy Li-Ion Batteries
journal, May 2018
- Wang, Fei; Borodin, Oleg; Ding, Michael S.
- Joule, Vol. 2, Issue 5
Anion Hosting Cathodes in Dual-Ion Batteries
journal, July 2017
- Rodríguez-Pérez, Ismael A.; Ji, Xiulei
- ACS Energy Letters, Vol. 2, Issue 8
Current research trends and prospects among the various materials and designs used in lithium-based batteries
journal, February 2013
- Wagner, Ralf; Preschitschek, Nina; Passerini, Stefano
- Journal of Applied Electrochemistry, Vol. 43, Issue 5
All-Organic Rechargeable Battery with Reversibility Supported by “Water-in-Salt” Electrolyte
journal, January 2017
- Dong, Xiaoli; Yu, Hongchuan; Ma, Yuanyuan
- Chemistry - A European Journal, Vol. 23, Issue 11
Recent Progress in Aqueous Lithium-Ion Batteries
journal, June 2012
- Wang, Yonggang; Yi, Jin; Xia, Yongyao
- Advanced Energy Materials, Vol. 2, Issue 7
Before Li Ion Batteries
journal, November 2018
- Winter, Martin; Barnett, Brian; Xu, Kang
- Chemical Reviews, Vol. 118, Issue 23
Rechargeable Lithium Batteries with Aqueous Electrolytes
journal, May 1994
- Li, W.; Dahn, J. R.; Wainwright, D. S.
- Science, Vol. 264, Issue 5162, p. 1115-1118
Li + Ion Insertion in TiO 2 (Anatase). 2. Voltammetry on Nanoporous Films
journal, September 1997
- Lindström, Henrik; Södergren, Sven; Solbrand, Anita
- The Journal of Physical Chemistry B, Vol. 101, Issue 39
Enabling bis(fluorosulfonyl)imide-based ionic liquid electrolytes for application in dual-ion batteries
journal, January 2018
- Beltrop, Kolja; Qi, Xin; Hering, Tobias
- Journal of Power Sources, Vol. 373
Anion intercalation into highly oriented pyrolytic graphite studied by electrochemical atomic force microscopy
journal, January 1999
- Alliata, D.; Häring, P.; Haas, O.
- Electrochemistry Communications, Vol. 1, Issue 1
Rechargeable Dual‐Ion Batteries with Graphite as a Cathode: Key Challenges and Opportunities
text, January 2019
- V., Kravchyk, Kostiantyn; V., Kovalenko, Maksym
- ETH Zurich
Fluorine-free water-in-ionomer electrolytes for sustainable lithium-ion batteries
text, January 2018
- He, Xin; Yan, Bo; Zhang, Xin
- Karlsruhe
Hybrid Aqueous/Non-aqueous Electrolyte for Safe and High-Energy Li-Ion Batteries
journal, October 2018
- Wang, Fei; Borodin, Oleg; Ding, Michael S.
- Joule, Vol. 2, Issue 10
Intercalation compounds of graphite
journal, April 1981
- Dresselhaus, M. S.; Dresselhaus, G.
- Advances in Physics, Vol. 30, Issue 2
Advanced High-Voltage Aqueous Lithium-Ion Battery Enabled by “Water-in-Bisalt” Electrolyte
journal, April 2016
- Suo, Liumin; Borodin, Oleg; Sun, Wei
- Angewandte Chemie, Vol. 128, Issue 25