Progress in electrolytes for beyond-lithium-ion batteries

doi:10.1016/j.jmst.2020.01.017

Abstract

Abstract:

The constant increase in global energy demand and stricter environmental standards are calling for advanced energy storage technologies that can store electricity from intermittent renewable sources such as wind, solar, and tidal power, to allow the broader implementation of the renewables. The grid-oriented sodium-ion batteries, potassium ion batteries and multivalent ion batteries are cheaper and more sustainable alternatives to Li-ion, although they are still in the early stages of development. Additional optimisation of these battery systems is required, to improve the energy and power density, and to solve the safety issues caused by dendrites growth in anodes. Electrolyte, one of the most critical components in these batteries, could significantly influence the electrochemical performances and operations of batteries. In this review, the definitions and influences of three critical components (salts, solvents, and additives) in electrolytes are discussed. The significant advantages, challenges, recent progress and future optimisation directions of various electrolytes for monovalent and multivalent ions batteries (i.e. organic, ionic liquid and aqueous liquid electrolytes, polymer and inorganic solid electrolytes) are summarised to guide the practical application for grid-oriented batteries.

Key words: Electrolytes, Organic liquid electrolyte, Aqueous electrolyte, Ionic liquid electrolyte, Solid-state electrolyte, Sodium-ion batteries, Potassium ion batteries, Multivalent ion batteries

Juyan Zhang, Xuhui Yao, Ravi K. Misra, Qiong Cai, Yunlong Zhao. Progress in electrolytes for beyond-lithium-ion batteries[J]. J. Mater. Sci. Technol., 2020, 44: 237-257.

Figures/Tables 12

Fig. 1. Characteristics of promising grid-oriented batteries. (a) Elemental abundance of Li, Na, K, Mg, Ca, Zn, Al in the earth’s crust; (b) Theoretical specific and volumetric capacity of Li, Na, K, Mg, Ca, Zn, Al-metal anodes; the larger capacity (vs. Li) is due to the higher number of electrons involved in the electrochemical process. (c) Representative operational voltage and discharge specific capacity of recently developed battery systems and the types of electrolyte applied.

Fig. 2. (a) Composition and design principle of conventional liquid electrolytes. (b) Different physical and electrochemical characteristics of electrolytes. The height of the rectangle represents the weight of the influence of these factors: metal salts (blue), solvent (red) and additives (green).

Table 1 General properties of commonly used polymer hosts and their advantages and disadvantages.

Polymer host	Ionic conductivity at room temperature (S cm^-1)	Advantages	Disadvantages	Refs.
PEO	2.6×10-4	Good dimensional stability; high capacity in salt complexation; high ionic conductivity in the amorphous state; good corrosion resistance; acceptable commercial cost; mechanical flexibility and chemical stability	Low ionic conductivity at ambient temperature; loss of dimensional stability above melting point; relative high degree of crystallisation	[185,186]
PVdF	4.5×10-3	Good affinity to electrolyte solution; good electrochemical stability; high dielectric constant; high anodic stability	Hindered ions transport by crystalline part (high degree of crystallinity) and caused low charge/discharge capacities	[187,188,189]
PVdF-HFP	4.3×10-3	High ionic conductivity; good mechanical strength	Poor compatibility of the LiBF₄ with the lithium anode	[190,191]
PMMA	7.3×10-6	Low mechanical integrity; high brittleness	Its proportion significantly influence the viscosity and cause low ionic conductivity	[192,193]
PVC	2.83×10-6	Low cost; good compatibility with most of the additives	Low ionic conductivity at room temperature	[194]
PVA	4.75×10-2	Good tensile and mechanical strength; non-toxicity; cost-effectiveness; good optical properties; high-temperature resistance and high hydrophilicity; good flexibility; biocompatibility; excellent chemical and thermal stabilities; high dielectric constant		[195,196]
PAA	2.15×10-4	Superior mechanical strength; good processability; biodegradability; environmentally friendly		[197]
PAN	5.7×10-4	High thermal stability; high ionic conductivity; good morphology for electrolyte; mechanical stability; minimisation of dendrite growth	Poor compatibility with lithium metal anode (lead to poor cyclability and safety hazards)	[198,199]

Table 1 General properties of commonly used polymer hosts and their advantages and disadvantages.

Polymer host	Ionic conductivity at room temperature (S cm^-1)	Advantages	Disadvantages	Refs.
PEO	2.6×10-4	Good dimensional stability; high capacity in salt complexation; high ionic conductivity in the amorphous state; good corrosion resistance; acceptable commercial cost; mechanical flexibility and chemical stability	Low ionic conductivity at ambient temperature; loss of dimensional stability above melting point; relative high degree of crystallisation	[185,186]
PVdF	4.5×10-3	Good affinity to electrolyte solution; good electrochemical stability; high dielectric constant; high anodic stability	Hindered ions transport by crystalline part (high degree of crystallinity) and caused low charge/discharge capacities	[187,188,189]
PVdF-HFP	4.3×10-3	High ionic conductivity; good mechanical strength	Poor compatibility of the LiBF₄ with the lithium anode	[190,191]
PMMA	7.3×10-6	Low mechanical integrity; high brittleness	Its proportion significantly influence the viscosity and cause low ionic conductivity	[192,193]
PVC	2.83×10-6	Low cost; good compatibility with most of the additives	Low ionic conductivity at room temperature	[194]
PVA	4.75×10-2	Good tensile and mechanical strength; non-toxicity; cost-effectiveness; good optical properties; high-temperature resistance and high hydrophilicity; good flexibility; biocompatibility; excellent chemical and thermal stabilities; high dielectric constant		[195,196]
PAA	2.15×10-4	Superior mechanical strength; good processability; biodegradability; environmentally friendly		[197]
PAN	5.7×10-4	High thermal stability; high ionic conductivity; good morphology for electrolyte; mechanical stability; minimisation of dendrite growth	Poor compatibility with lithium metal anode (lead to poor cyclability and safety hazards)	[198,199]

Table 2 Compositions of recently widely reported different types of electrolytes for different metal ion batteries.

Electrolyte types	Battery types	Electrolyte compositions			Refs.
Electrolyte types	Battery types	Salts	Solvents	Additives	Refs.
Non-aqueous organic liquid electrolytes	NIBs	NaPF₆, NaClO₄, NaTFSI, NaFSI, NaFTSI, NaCF₃SO₃	EC, PC, EMC, DEC, DMC, DME, Triglyme, PC:EMC (1:1 vol.%), EC:DMC (2:1 wt%), EC:PC:DMC (45:45:10 vol%), EC:PC (1:1 vol.%), EC:DEC (1:1 wt%) EC:DME (1:1 wt%), Ec:triglyme (1:1 wt%)	FEC FEC-PST, FEC-PST-DTD SiO₂-IL-ClO₄ FEC, InI₃	[28,31,52,62,97]
	KIBs	KPF₆, KFSA, KTFSA, KFSI	PC, DME, GBL, diglyme TMP		[16,115,116,117,121]
	MIBs	HMDSMgCl, Mg[B(hfip)₄]₂, Mg(HMDS) ₂, [Mg(DG)₂][HMDSAlCl₃]₂, Mg(TFSI)₂	THF, diglyme, tetraglyme, DME	DEME?TFSIMgCl₂, AlCl₃	[43,129,130,131,132,138,139,140,141,200]
	AIBs	Dialkylsufones-AlCl₃ (EiPS, EnPS, DnPS or EsBS)	toluene		[162]
	CIBs	Ca(BF₄)₂, Ca(PF₄)₂, Ca(BH₄)₂	EC:PC(1:1 wt%) EC:PC:DMC:EMC (2:2:3:3 vol.%), THF		[11,19,184]
Aqueous liquid electrolytes	KIBs	Potassium acetate (KAc)	H₂O		[118]
	ZIBs	ZnSO₄, Zn(CF₃SO₃)₂	H₂O	MnSO₂	[68,174,176]
	CIBs	Ca(NO₃)₂, Ca(ClO₄)₂, Ca(TFSI)₂, Ca(PF₆)₂	H₂O		[34,35]
Ionic liquid electrolytes	NIBs	NaBr -NaAlCl₄, NaFSA-KFSA, BMPTFSI- NaClO₄, EMIBF₄- NaBF₄, (Pyr₁₄TFSI)-NaFTSI		EC:PC EC	[55,77,99,100,101,102]
	MIBs	MgCl₃-AlCl₃		Mg	[201]
	AIBs	MCl-AlCl₃ (M = Li⁺, Na⁺, K⁺, [BMIM]⁺, [EMIm]⁺, Et₃NH			[58,163,164,169,202]
	ZIBs	LiTFSI -Zn(Tfo)₂, ZnBr₂-KI			[182]
Solid electrolytes	NIBs	NaClO₄, Na_2-x(CB₁₁H₁₂)_x(B₁₂H₁₂)_1-x	P(VdF-co-HFP), PMA-PEG		[107,108,111]
	MIBs	Mg(ClO₄)₂	PVdF-HFP, PEC, PVAc		[127,128]
	AIBs	[EMIm]Cl-AlCl₃	acrylamide		[203]

Fig. 3. (a) Conductivity (black bars and left-hand side y-axis) and viscosity (green bars and right-hand side y-axis) values of electrolytes based on 1 M NaClO4 dissolved in various solvents and solvent mixtures; (b) Electrochemical potential window stability (black bars and upper y-axis) and thermal range (green bars and lower y-axis) values of: PC based electrolytes with 1 M of various Na salts (top) and electrolytes based on 1 M NaClO4 dissolved in various solvents and solvent mixtures (bottom), reprinted from Ref. [31] with permission; (c) Na/S @MPCF cells containing 2 M NaTFSI in PC:FEC solvent with various FEC proportion and with/without InI3, reprinted from Ref. [97] with permission; (d) Electrochemical stability windows of the CPE measured by LSV at 0.1 V s-1, reprinted from Ref. [107] with permission; (e) Schematic summary on the role of PST and DTD additives in HC/NFM full cell, reprinted from Ref [62]. with permission; (f) Galvanostatic voltage profile of Na-Sn|Na4/3(CB11H12)2/3(B12H12)1/3|Na-Sn cell, reprinted from Ref. [111] with permission.

Fig. 4. (a) Molality vs. ionic conductivity plots of KFSA in DME, GBL and PC, and KTFSA/DME solutions measured at 28 °C, reprinted from Ref. [16] with permission; (b) Cycling performance of graphite anode in different salt-concentration electrolytes KFSI-DME at a current rate of 0.5 C (1 C corresponds to 280 mA h g-1), reprinted from Ref. [115] with permission; (c) Flammability tests in 1 M KPF6/EC-DEC electrolyte (left side) and 3.3 M KFSI/TMP electrolyte (right side) reprinted from Ref. [117] with permission; (d) The graphite anodes storage potassium mechanism in different salt concentrations. Between 3 mol/kg and 7 mol/kg, it is a combination of K+ and [K-DMEx]+ co-insertion behaviour, reprinted from Ref. [115] with permission; (e) Linear voltammetry curves recorded at 1 mV/s in 1 M, 10 M, 30 M KAc electrolyte reprinted from Ref [118]. with permission.

Fig. 5. (a) Cyclic voltammograms for THF-based electrolyte of Mg(HMDS)2 complexed with AlCl3, reprinted from Ref. [130] with permission; Cyclic voltammograms with Pt electrodes of THF solution containing Mg(HMDS)2 and MgCl2 in the different ratio: (b) 0.5 M 2 Mg(HMDS)2 - MgCl2; (c) 0.5 M Mg(HMDS)2 2 MgCl2; (d) 0.5 M Mg(HMDS)2-4MgCl2; reprinted from Ref. [131] with permission; (e) ionic conductivity of 0.625 M solutions of Mg(HMDS)2-MgCl2 in THF containing a different concentration of DEME/TFSI; reprinted from Ref. [132] with permission; (f) Cycling behaviour of a symmetrical cell with electrolyte [Mg(DG)2][(HMDSAlCl3)]2-DG from 50 μA cm-2 to 5 mA cm-2. Reprinted from Ref. [133] with permission; (g) cyclic voltammograms for MMAC-DME electrolyte with in situ Mg powder (red) and without Mg treatment (black); reprinted from Ref. [134] with permission; the cycling efficiencies and selected voltage profiles (inset) of (h) 0.5 M Mg(TFSI)2 + 0.15 M Mg[B(OPh)3H]2 in diglyme; (i) 0.5 M Mg(TFSI)2 + 0.15 M Mg[B(OPh)3H]2 + 0.1 M MgCl2 in diglyme; reprinted from Ref. [140]with permission.

Fig. 6. Scheme of the proposed degradation mechanisms of Mg metal anodes at high current density; Optical images of a Mg metal anode and the electrolyte, reprinted from Ref. [138] with permission.

Fig. 7. (a) HOMO and LUMO plots of [EMIm]+AlCl4- and [Et3NH]+AlCl4- calculated by DFT. reprinted from Ref. [165] with permission; (b) Cyclic voltammogram of AlCl3/[BMIM]Cl ionic liquids with different mole ratios; (c) SEM images of Al metal foil immersed in AlCl3/[BMIM]Cl ionic liquid s with different mole ratios for 24 h: (1) initial; (2) 0.8:1; (3) 1:1; (4) 1.1:1; (5) 1.5:1; and (6) 2:1. reprinted from Ref. [163] with permission.

Fig. 8. (a) The CV of Zn/MnO2 batteries in with and without 0.1 M MnSO4 additive in a 2 M ZnSO4 aqueous electrolyte at C/3 and 1 C, respectively; (b) The long-term cyclic performance of Zn/MnO2 battery using an electrolyte with a MnSO4 additive. Reprinted from Ref. [68] with permission; (c) Schematic showing the structure of gum Zn-MnO2 battery; (d) SEM image of the MnO2/CNT hybrid film; Reprinted from Ref. [175] with permission; (e) Cyclic voltammograms of Zn electrode in aqueous electrolyte of (e) 1 M Zn(CF3SO3)2 and (f) 1 M ZnSO4 at the scan rate of 0.5 mV s-1 between -0.2 and 2.0 V; Reprinted from Ref. [177] with permission; (g) Illustration of the overcharging and self-healing process. Reprinted from Ref [182]. with permission.

Fig. 9. (a) Work schematics of the proposed CIB; (b) Corresponding dQ/dV curve of the charge-discharge profile; (c) X-ray diffraction; Reprinted from Ref. [19] with permission; Electrochemical results of calcium plating/stripping in 1.5 M Ca(BH4)2 in THF; (d) Cyclic voltammogram of calcium plating/stripping; (e) Galvanostatic calcium plating/stripping at a rate of 1 mA cm-2 Reprinted from Ref. [184] with permission.

Fig. 10. The special properties of various types of electrolytes, as well as their future work, and the mean development fields of different types of metal ion batteries in the future.

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