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Advances and issues in developing salt-concentrated battery electrolytes

A Publisher Correction to this article was published on 26 March 2019

This article has been updated

Abstract

With a worldwide trend towards the efficient use of renewable energies and the rapid expansion of the electric vehicle market, the importance of rechargeable battery technologies, particularly lithium-ion batteries, has steadily increased. In the past few years, a major breakthrough in electrolyte materials was achieved by simply increasing the salt concentration in suitable salt–solvent combinations, offering technical superiority in numerous figures of merit over alternative materials. This long-awaited, extremely simple yet effective strategy can overcome most of the remaining hurdles limiting the present lithium-ion batteries without sacrificing manufacturing efficiency, and hence its impact is now widely felt in the scientific community, with serious potential for industrial development. This Review aims to provide timely and objective information that will be valuable for designing better realistic batteries, including a multi-angle analysis of their advantages and disadvantages together with future perspectives. Emphasis is placed on the pathways to address the remaining technical and scientific issues rather than re-highlighting the many technical advantages.

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Fig. 1: Overview of a conventional dilute electrolyte and salt-concentrated electrolyte.
Fig. 2: Advanced battery functions realized by concentrated electrolytes.
Fig. 3: Mechanism of ion transport.
Fig. 4: Diluting concentrated electrolytes with a low-polarity solvent.
Fig. 5: SEI formation process in a concentrated electrolyte.
Fig. 6: Computational methodologies for electrolyte analyses.
Fig. 7: Multi-angle comparison of three types of electrolyte.

Change history

  • 26 March 2019

    An amendment to this paper has been published and can be accessed via a link at the top of the paper.

References

  1. 1.

    Xu, K. Nonaqueous liquid electrolytes for lithium-based rechargeable batteries. Chem. Rev. 104, 4303–4417 (2004).

    Google Scholar 

  2. 2.

    Fong, R., von Sacken, U. & Dahn, J. R. Studies of lithium intercalation into carbons using nonaqueous electrochemical cells. J. Electrochem. Soc. 137, 2009–2013 (1990).

    Google Scholar 

  3. 3.

    Myung, S.-T., Sasaki, Y., Sakurada, S., Sun, Y.-K. & Yashiro, H. Electrochemical behavior of current collectors for lithium batteries in non-aqueous alkyl carbonate solution and surface analysis by ToF-SIMS. Electrochim. Acta 55, 288–297 (2009).

    Google Scholar 

  4. 4.

    Xu, K. Electrolytes and interphases in Li-ion batteries and beyond. Chem. Rev. 114, 11503–11618 (2014).

    Google Scholar 

  5. 5.

    Wang, D. Y. et al. A systematic study of electrolyte additives in Li[Ni1/3Mn1/3Co1/3]O2 (NMC)/graphite pouch cells. J. Electrochem. Soc. 161, A1818–A1827 (2014).

    Google Scholar 

  6. 6.

    Watanabe, M. et al. Application of ionic liquids to energy storage and conversion materials and devices. Chem. Rev. 117, 7190–7239 (2017).

    Google Scholar 

  7. 7.

    Hallinan, D. T. & Balsara, N. P. Polymer electrolytes. Annu. Rev. Mater. Res. 43, 503–525 (2013).

    Google Scholar 

  8. 8.

    Janek, J. & Zeier, W. G. A solid future for battery development. Nat. Energy 1, 16141 (2016).

    Google Scholar 

  9. 9.

    Manthiram, A., Yu, X. & Wang, S. Lithium battery chemistries enabled by solid-state electrolytes. Nat. Rev. Mater. 2, 16103 (2017).

    Google Scholar 

  10. 10.

    Yamada, Y. & Yamada, A. Review — superconcentrated electrolytes for lithium batteries. J. Electrochem. Soc. 162, A2406–A2423 (2015).

    Google Scholar 

  11. 11.

    Zheng, J., Lochala, J. A., Kwok, A., Deng, Z. D. & Xiao, J. Research progress towards understanding the unique interfaces between concentrated electrolytes and electrodes for energy storage applications. Adv. Sci. 4, 1700032 (2017).

    Google Scholar 

  12. 12.

    Yoshida, K. et al. Oxidative-stability enhancement and charge transport mechanism in glyme-lithium salt equimolar complexes. J. Am. Chem. Soc. 133, 13121–13129 (2011). This work reported enhanced oxidation stability of concentrated electrolytes and clarified the mechanism (the downward sihft of HOMO).

    Google Scholar 

  13. 13.

    Seo, D. M., Borodin, O., Han, S.-D., Boyle, P. D. & Henderson, W. A. Electrolyte solvation and ionic association II. Acetonitrile-lithium salt mixtures: highly dissociated salts. J. Electrochem. Soc. 159, A1489–A1500 (2012).

    Google Scholar 

  14. 14.

    Yamada, Y. et al. Unusual stability of acetonitrile-based superconcentrated electrolytes for fast-charging lithium-ion batteries. J. Am. Chem. Soc. 136, 5039–5046 (2014). This work reported enhanced reduction stability of concentrated electrolytes and clarified the mechanism (anion-derived SEI formation).

    Google Scholar 

  15. 15.

    Yamada, Y. et al. General observation of lithium intercalation into graphite in ethylene-carbonate-free superconcentrated electrolytes. ACS Appl. Mater. Interfaces 6, 10892–10899 (2014).

    Google Scholar 

  16. 16.

    McOwen, D. W. et al. Concentrated electrolytes: decrypting electrolyte properties and reassessing Al corrosion mechanisms. Energy Environ. Sci. 7, 416–426 (2014).

    Google Scholar 

  17. 17.

    Zhang, C. et al. Chelate effects in glyme/lithium bis(trifluoromethanesulfonyl)amide solvate ionic liquids, part 2: importance of solvate-structure stability for electrolytes of lithium batteries. J. Phys. Chem. C 118, 17362–17373 (2014).

    Google Scholar 

  18. 18.

    Yamada, Y., Yaegashi, M., Abe, T. & Yamada, A. A superconcentrated ether electrolyte for fast-charging Li-ion batteries. Chem. Commun. 49, 11194 (2013).

    Google Scholar 

  19. 19.

    Petibon, R., Aiken, C. P., Ma, L., Xiong, D. & Dahn, J. R. The use of ethyl acetate as a sole solvent in highly concentrated electrolyte for Li-ion batteries. Electrochim. Acta 154, 287–293 (2015).

    Google Scholar 

  20. 20.

    Wang, J. et al. Superconcentrated electrolytes for a high-voltage lithium-ion battery. Nat. Commun. 7, 12032 (2016). This work demonstrated the reversible operation of 5 V-class batteries with concentrated electrolytes.

    Google Scholar 

  21. 21.

    Wang, J. et al. Fire-extinguishing organic electrolytes for safe batteries. Nat. Energy 3, 22–29 (2018). This work presented non-flammable and fire-extinguishing organic electrolytes that enabled long-term battery cycling.

    Google Scholar 

  22. 22.

    Choi, J. W. & Aurbach, D. Promise and reality of post-lithium-ion batteries with high energy densities. Nat. Rev. Mater. 1, 16013 (2016).

    Google Scholar 

  23. 23.

    Aurbach, D. et al. Review on electrode–electrolyte solution interactions, related to cathode materials for Li-ion batteries. J. Power Sources 165, 491–499 (2007).

    Google Scholar 

  24. 24.

    Kim, J.-H. et al. Understanding the capacity fading mechanism in LiNi0.5Mn1.5O4/graphite Li-ion batteries. Electrochim. Acta 90, 556–562 (2013).

    Google Scholar 

  25. 25.

    Wang, X., Yasukawa, E. & Mori, S. Inhibition of anodic corrosion of aluminum cathode current collector on recharging in lithium imide electrolytes. Electrochim. Acta 45, 2677–2684 (2000).

    Google Scholar 

  26. 26.

    Li, L. et al. Transport and electrochemical properties and spectral features of non-aqueous electrolytes containing LiFSI in linear carbonate solvents. J. Electrochem. Soc. 158, A74–A82 (2011).

    Google Scholar 

  27. 27.

    Matsumoto, K. et al. Suppression of aluminum corrosion by using high concentration LiTFSI electrolyte. J. Power Sources 231, 234–238 (2013). This work demonstrated the corrosion prevention of an Al current collector in concentrated electrolytes.

    Google Scholar 

  28. 28.

    Suo, L., Hu, Y.-S., Li, H., Armand, M. & Chen, L. A new class of solvent-in-salt electrolyte for high-energy rechargeable metallic lithium batteries. Nat. Commun. 4, 1481 (2013). This work reported less solubility of lithium polysulfide in concentrated electrolytes to achieve better cycling of lithium-sulfur batteries.

    Google Scholar 

  29. 29.

    Dokko, K. et al. Solvate ionic liquid electrolyte for Li-S batteries. J. Electrochem. Soc. 160, A1304–A1310 (2013). This work reported the dilution of concentrated electrolytes with low-polar solvent that could retain unusual functions of original concentrated electrolytes with lower viscosity and higher ionic conductivity.

    Google Scholar 

  30. 30.

    Jiao, S. et al. Stable cycling of high-voltage lithium metal batteries in ether electrolytes. Nat. Energy 3, 739–746 (2018).

    Google Scholar 

  31. 31.

    Jeong, S. K. et al. Suppression of dendritic lithium formation by using concentrated electrolyte solutions. Electrochem. Commun. 10, 635–638 (2008). This work applied the concept of concentrated electrolytes to lithium metal anodes to achieve better Coulombic efficiencies and less dendritic deposition.

    Google Scholar 

  32. 32.

    Qian, J. et al. High rate and stable cycling of lithium metal anode. Nat. Commun. 6, 6362 (2015).

    Google Scholar 

  33. 33.

    Tatara, R. et al. Solvate ionic liquid, [Li(triglyme)1][NTf2], as electrolyte for rechargeable Li/air battery: discharge depth and reversibility. Chem. Lett. 42, 1053–1055 (2013).

    Google Scholar 

  34. 34.

    Li, F., Zhang, T., Yamada, Y., Yamada, A. & Zhou, H. Enhanced cycling performance of Li-O2 batteries by the optimized electrolyte concentration of LiTFSA in glymes. Adv. Energy Mater. 3, 532–538 (2013).

    Google Scholar 

  35. 35.

    He, M. et al. Concentrated electrolyte for the sodium-oxygen battery: solvation structure and improved cycle life. Angew. Chem. Int. Ed. 55, 15310–15314 (2016).

    Google Scholar 

  36. 36.

    Liu, B. et al. Enhanced cycling stability of rechargeable Li-O2 batteries using high-concentration electrolytes. Adv. Funct. Mater. 26, 605–613 (2016).

    Google Scholar 

  37. 37.

    Liu, B. et al. Stabilization of Li metal anode in DMSO-based electrolytes via optimization of salt–solvent coordination for Li–O2 batteries. Adv. Energy Mater. 7, 1602605 (2017).

    Google Scholar 

  38. 38.

    Okuoka, S. et al. A new sealed lithium-peroxide battery with a Co-doped Li2O cathode in a superconcentrated lithium bis(fluorosulfonyl)amide electrolyte. Sci. Rep. 4, 5684 (2014).

    Google Scholar 

  39. 39.

    Mogensen, R., Brandell, D. & Younesi, R. Solubility of the solid electrolyte interphase (SEI) in sodium ion batteries. ACS Energy Lett. 1, 1173–1178 (2016).

    Google Scholar 

  40. 40.

    Ribière, P. et al. Investigation on the fire-induced hazards of Li-ion battery cells by fire calorimetry. Energy Environ. Sci. 5, 5271–5280 (2012).

    Google Scholar 

  41. 41.

    Ping, P. et al. Study of the fire behavior of high-energy lithium-ion batteries with full-scale burning test. J. Power Sources 285, 80–89 (2015).

    Google Scholar 

  42. 42.

    Wang, X., Yasukawa, E. & Kasuya, S. Nonflammable trimethyl phosphate solvent-containing electrolytes for lithium-ion batteries: I. fundamental properties. J. Electrochem. Soc. 148, A1058–A1065 (2001).

    Google Scholar 

  43. 43.

    Matsumoto, K. et al. Performance improvement of Li ion battery with non-flammable TMP mixed electrolyte by optimization of lithium salt concentration and SEI preformation technique on graphite anode. J. Electrochem. Soc. 161, A831–A834 (2014).

    Google Scholar 

  44. 44.

    Zeng, Z. et al. A safer sodium-ion battery based on nonflammable organic phosphate electrolyte. Adv. Sci. 3, 1600066 (2016).

    Google Scholar 

  45. 45.

    Hess, S., Wohlfahrt-Mehrens, M. & Wachtler, M. Flammability of Li-ion battery electrolytes: flash point and self-extinguishing time measurements. J. Electrochem. Soc. 162, A3084–A3097 (2015).

    Google Scholar 

  46. 46.

    Zeng, Z. et al. Non-flammable electrolytes with high salt-to-solvent ratios for Li-ion and Li-metal batteries. Nat. Energy 3, 674–681 (2018).

    Google Scholar 

  47. 47.

    Suo, L. et al. ‘Water-in-salt’ electrolyte enables high-voltage aqueous lithium-ion chemistries. Science 350, 938–943 (2015). This work applied the concept of concentrated electrolytes to an aqueous system to achieve high-voltage aqueous batteries.

    Google Scholar 

  48. 48.

    Yamada, Y. et al. Hydrate-melt electrolytes for high-energy-density aqueous batteries. Nat. Energy 1, 16129 (2016).

    Google Scholar 

  49. 49.

    Yang, C. et al. 4.0 V aqueous Li-ion batteries. Joule 1, 122–132 (2017).

    Google Scholar 

  50. 50.

    Zheng, H., Li, J., Song, X., Liu, G. & Battaglia, V. S. A comprehensive understanding of electrode thickness effects on the electrochemical performances of Li-ion battery cathodes. Electrochim. Acta 71, 258–265 (2012).

    Google Scholar 

  51. 51.

    Sander, J. S., Erb, R. M., Li, L., Gurijala, A. & Chiang, Y.-M. High-performance battery electrodes via magnetic templating. Nat. Energy 1, 16099 (2016).

    Google Scholar 

  52. 52.

    Takada, K. et al. Unusual passivation ability of superconcentrated electrolytes toward hard carbon negative electrodes in sodium-ion batteries. ACS Appl. Mater. Interfaces 9, 33802–33809 (2017).

    Google Scholar 

  53. 53.

    Aihara, Y., Sugimoto, K., Price, W. S. & Hayamizu, K. Ionic conduction and self-diffusion near infinitesimal concentration in lithium salt-organic solvent electrolytes. J. Chem. Phys. 113, 1981–1991 (2000).

    Google Scholar 

  54. 54.

    Tang, Z. K., Tse, J. S. & Liu, L. M. Unusual Li-ion transfer mechanism in liquid electrolytes: a first-principles study. J. Phys. Chem. Lett. 7, 4795–4801 (2016).

    Google Scholar 

  55. 55.

    Okoshi, M., Chou, C. P. & Nakai, H. Theoretical analysis of carrier ion diffusion in superconcentrated electrolyte solutions for sodium-ion batteries. J. Phys. Chem. B 122, 2600–2609 (2018).

    Google Scholar 

  56. 56.

    Borodin, O. et al. Liquid structure with nano-heterogeneity promotes cationic transport in concentrated electrolytes. ACS Nano 11, 10462–10471 (2017).

    Google Scholar 

  57. 57.

    Ushirogata, K., Sodeyama, K., Futera, Z., Tateyama, Y. & Okuno, Y. Near-shore aggregation mechanism of electrolyte decomposition products to explain solid electrolyte interphase formation. J. Electrochem. Soc. 162, A2670–A2678 (2015).

    Google Scholar 

  58. 58.

    Jeong, S.-K., Inaba, M., Iriyama, Y., Abe, T. & Ogumi, Z. Electrochemical intercalation of lithium ion within graphite from propylene carbonate solutions. Electrochem. Solid State Lett. 6, A13–A15 (2003). This work discovered unusual behaviour of concentrated electrolytes in lithium-ion batteries.

    Google Scholar 

  59. 59.

    Yamada, Y. et al. Corrosion prevention mechanism of aluminum metal in superconcentrated electrolytes. ChemElectroChem 2, 1687–1694 (2015).

    Google Scholar 

  60. 60.

    Alvarado, J. et al. A carbonate-free, sulfone-based electrolyte for high-voltage Li-ion batteries. Mater. Today 21, 341–353 (2018).

    Google Scholar 

  61. 61.

    Moon, H. et al. Solvent activity in electrolyte solutions controls electrochemical reactions in Li-ion and Li-sulfur batteries. J. Phys. Chem. C 6, 3957–3970 (2015).

    Google Scholar 

  62. 62.

    Ren, X. et al. Localized high-concentration sulfone electrolytes for high-efficiency lithium-metal batteries. Chem 4, 1877–1892 (2018).

    Google Scholar 

  63. 63.

    Ueno, K. et al. Li+ solvation and ionic transport in lithium solvate ionic liquids diluted by molecular solvents. J. Phys. Chem. C 120, 15792–15802 (2016).

    Google Scholar 

  64. 64.

    Chen, S. et al. High-voltage lithium-metal batteries enabled by localized high-concentration electrolytes. Adv. Mater. 1706102, 1706102 (2018).

    Google Scholar 

  65. 65.

    Doi, T., Shimizu, Y., Hashinokuchi, M. & Inaba, M. Dilution of highly concentrated LiBF4/propylene carbonate electrolyte solution with fluoroalkyl ethers for 5-V LiNi0.5Mn1.5O4 positive electrodes. J. Electrochem. Soc. 164, A6412–A6416 (2017).

    Google Scholar 

  66. 66.

    Yabuuchi, N., Kubota, K., Dahbi, M. & Komaba, S. Research development on sodium-ion batteries. Chem. Rev. 114, 11636–11682 (2014).

    Google Scholar 

  67. 67.

    Wu, X., Leonard, D. P. & Ji, X. Emerging non-aqueous potassium-ion batteries: challenges and opportunities. Chem. Mater. 29, 5031–5042 (2017).

    Google Scholar 

  68. 68.

    Erickson, E. M. et al. Review — development of advanced rechargeable batteries: a continuous challenge in the choice of suitable electrolyte solutions. J. Electrochem. Soc. 162, A2424–A2438 (2015).

    Google Scholar 

  69. 69.

    Elia, G. A. et al. An overview and future perspectives of aluminum batteries. Adv. Mater. 28, 7564–7579 (2016).

    Google Scholar 

  70. 70.

    Komaba, S. et al. Electrochemical Na insertion and solid electrolyte interphase for hard-carbon electrodes and application to Na-ion batteries. Adv. Funct. Mater. 21, 3859–3867 (2011).

    Google Scholar 

  71. 71.

    Ponrouch, A., Marchante, E., Courty, M., Tarascon, J.-M. & Palacín, M. R. In search of an optimized electrolyte for Na-ion batteries. Energy Environ. Sci. 5, 8572–8583 (2012).

    Google Scholar 

  72. 72.

    Eshetu, G. G. et al. Comprehensive insights into the reactivity of electrolytes based on sodium ions. ChemSusChem 9, 462–471 (2016).

    Google Scholar 

  73. 73.

    Jian, Z., Luo, W. & Ji, X. Carbon electrodes for K-ion batteries. J. Am. Chem. Soc. 137, 11566–11569 (2015).

    Google Scholar 

  74. 74.

    Komaba, S., Hasegawa, T., Dahbi, M. & Kubota, K. Potassium intercalation into graphite to realize high-voltage/high-power potassium-ion batteries and potassium-ion capacitors. Electrochem. Commun. 60, 172–175 (2015).

    Google Scholar 

  75. 75.

    Okoshi, M., Yamada, Y., Komaba, S., Yamada, A. & Nakai, H. Theoretical analysis of interactions between potassium ions and organic electrolyte solvents: a comparison with lithium, sodium, and magnesium ions. J. Electrochem. Soc. 164, A54–A60 (2017).

    Google Scholar 

  76. 76.

    Aurbach, D. et al. Prototype systems for rechargeable magnesium batteries. Nature 407, 724–727 (2000).

    Google Scholar 

  77. 77.

    Cheng, Y. et al. Highly active electrolytes for rechargeable Mg batteries based on a [Mg2(μ-Cl)2]2+ cation complex in dimethoxyethane. Phys. Chem. Chem. Phys. 17, 13307–13314 (2015).

    Google Scholar 

  78. 78.

    Lin, M. C. et al. An ultrafast rechargeable aluminium-ion battery. Nature 520, 325–328 (2015).

    Google Scholar 

  79. 79.

    Huang, F. et al. Enhancing metallic lithium battery performance by tuning the electrolyte solution structure. J. Mater. Chem. A 6, 1612–1620 (2018).

    Google Scholar 

  80. 80.

    Chen, F. & Forsyth, M. Elucidation of transport mechanism and enhanced alkali ion transference numbers in mixed alkali metal–organic ionic molten salts. Phys. Chem. Chem. Phys. 18, 19336–19344 (2016).

    Google Scholar 

  81. 81.

    Ding, M. S., Von Cresce, A. & Xu, K. Conductivity, viscosity, and their correlation of a super-concentrated aqueous electrolyte. J. Phys. Chem. C 121, 2149–2153 (2017).

    Google Scholar 

  82. 82.

    Sodeyama, K., Yamada, Y., Aikawa, K., Yamada, A. & Tateyama, Y. Sacrificial anion reduction mechanism for electrochemical stability improvement in highly concentrated Li-salt electrolyte. J. Phys. Chem. C 118, 14091–14097 (2014).

    Google Scholar 

  83. 83.

    Yamada, Y. & Yamada, A. Superconcentrated electrolytes to create new interfacial chemistry in non-aqueous and aqueous rechargeable batteries. Chem. Lett. 46, 1056–1064 (2017).

    Google Scholar 

  84. 84.

    Suo, L. et al. Fluorine-donating electrolytes enable highly reversible 5-V-class Li metal batteries. Proc. Natl Acad. Sci. USA 115, 1156–1161 (2018).

    Google Scholar 

  85. 85.

    Lee, J. et al. Ultraconcentrated sodium bis(fluorosulfonyl)imide-based electrolytes for high-performance sodium metal batteries. ACS Appl. Mater. Interfaces 9, 3723–3732 (2017).

    Google Scholar 

  86. 86.

    Takenaka, N. et al. Microscopic formation mechanism of solid electrolyte interphase film in lithium-ion batteries with highly concentrated electrolyte. J. Phys. Chem. C 122, 2564–2571 (2018).

    Google Scholar 

  87. 87.

    Peng, Q., Liu, H. & Ye, S. Adsorption of organic carbonate solvents on a carbon surface probed by sum frequency generation (SFG) vibrational spectroscopy. J. Electroanal. Chem. 800, 134–143 (2017).

    Google Scholar 

  88. 88.

    Leung, K. et al. Using atomic layer deposition to hinder solvent decomposition in lithium ion batteries: first-principles modeling and experimental studies. J. Am. Chem. Soc. 133, 14741–14754 (2011).

    Google Scholar 

  89. 89.

    Tuckerman, M. E., Marx, D. & Parinello, M. The natue and transport mechanism of hydrated hydroxide ions in aqueous solution. Nature 417, 925–929 (2002).

    Google Scholar 

  90. 90.

    Marx, D., Tuckerman, M. E., Hutter, J. & Parrinello, M. The nature of the hydrated excess proton in water. Nature 397, 601–604 (1998).

    Google Scholar 

  91. 91.

    Borodin, O. et al. Modeling insight into battery electrolyte electrochemical stability and interfacial structure. Acc. Chem. Res. 50, 2886–2894 (2017).

    Google Scholar 

  92. 92.

    Borodin, O. & Smith, G. D. Development of many-body polarizable force fields for Li-battery applications: 2. LiTFSI-doped oligoether, polyether, and carbonate-based electrolytes. J. Phys. Chem. B 110, 6293–6299 (2006).

    Google Scholar 

  93. 93.

    Kohagen, M. et al. Performance of quantum chemically derived charges and persistence of ion cages in ionic liquids. a molecular dynamics simulations study of 1-n-butyl-3-methylimidazolium bromide. J. Phys. Chem. B 115, 693–702 (2011).

    Google Scholar 

  94. 94.

    Takenaka, N., Suzuki, Y., Sakai, H. & Nagaoka, M. On electrolyte-dependent formation of solid electrolyte interphase film in lithium-ion batteries: strong sensitivity to small structural difference of electrolyte molecules. J. Phys. Chem. C 118, 10874–10882 (2014).

    Google Scholar 

  95. 95.

    Cuisinier, M. et al. Unique behaviour of nonsolvents for polysulphides in lithium–sulphur batteries. Energy Environ. Sci. 7, 2697–2705 (2014).

    Google Scholar 

  96. 96.

    Moon, H. et al. Mechanism of Li ion desolvation at the interface of graphite electrode and glyme–Li salt solvate ionic liquids. J. Phys. Chem. B 118, 20246–20256 (2014).

    Google Scholar 

  97. 97.

    Kim, H. et al. In situ formation of protective coatings on sulfur cathodes in lithium batteries with LiFSI-based organic electrolytes. Adv. Energy Mater. 5, 1401792 (2015).

    Google Scholar 

  98. 98.

    Doi, T., Masuhara, R., Hashinokuchi, M., Shimizu, Y. & Inaba, M. Concentrated LiPF6/PC electrolyte solutions for 5-V LiNi0.5Mn1.5O4 positive electrode in lithium-ion batteries. Electrochim. Acta 209, 219–224 (2016).

    Google Scholar 

  99. 99.

    Suo, L. et al. Advanced high-voltage aqueous lithium-ion battery enabled by ‘water-in-bisalt’ electrolyte. Angew. Chem. Int. Ed. 55, 7136–7141 (2016).

    Google Scholar 

  100. 100.

    Lu, D. et al. Formation of reversible solid electrolyte interface on graphite surface from concentrated electrolytes. Nano Lett. 17, 1602–1609 (2017).

    Google Scholar 

  101. 101.

    Shiga, T., Kato, Y., Kondo, H. & Okuda, C. Self-extinguishing electrolytes using fluorinated alkyl phosphates for lithium batteries. J. Mater. Chem. A 5, 5156–5162 (2017).

    Google Scholar 

  102. 102.

    Yang, C. et al. Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility. Proc. Natl Acad. Sci. USA 114, 6197–6202 (2017).

    Google Scholar 

  103. 103.

    Fan, X. et al. Highly fluorinated interphases enable high-voltage Li-metal batteries. Chem 4, 174–185 (2018).

    Google Scholar 

  104. 104.

    Zheng, J. et al. Extremely stable sodium metal batteries enabled by localized high-concentration electrolytes. ACS Energy Lett. 3, 315–321 (2018).

    Google Scholar 

  105. 105.

    Wang, F. et al. Highly reversible zinc metal anode for aqueous batteries. Nat. Mater. 17, 543–549 (2018).

    Google Scholar 

  106. 106.

    Chen, S. et al. High-efficiency lithium metal batteries with fire-retardant electrolytes. Joule 2, 1548–1558 (2018).

    Google Scholar 

  107. 107.

    Tamura, T. et al. New glyme-cyclic imide lithium salt complexes as thermally stable electrolytes for lithium batteries. J. Power Sources 195, 6095–6100 (2010).

    Google Scholar 

  108. 108.

    Yamada, Y., Takazawa, Y., Miyazaki, K. & Abe, T. Electrochemical lithium intercalation into graphite in dimethyl sulfoxide-based electrolytes: effect of solvation structure of lithium ion. J. Phys. Chem. C 114, 11680–11685 (2010).

    Google Scholar 

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Yamada, Y., Wang, J., Ko, S. et al. Advances and issues in developing salt-concentrated battery electrolytes. Nat Energy 4, 269–280 (2019). https://doi.org/10.1038/s41560-019-0336-z

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