电解液调控策略提升水系锌离子电池正极材料电化学性能

doi:10.3866/PKU.WHXB202205045

Abstract

Abstract:

The ever-worsening world-wide energy crisis and environmental issues are encouraging the development of green and renewable energy. Thus, rechargeable batteries are being developed and employed for energy storage and conversion in various electronic equipment. When compared with metal lithium batteries, aqueous rechargeable batteries have gained significant attention due to their advantages of high safety, low cost, and environmental friendliness. Among the various known rechargeable batteries (Li⁺, Na⁺, K⁺, NH₄⁺, Mg²⁺, Ca²⁺, and Al³⁺), aqueous zinc-ion batteries (ZIBs) are considered as promising energy storage devices because the zinc electrode exhibits high capacity (820 mAh∙g⁻¹) and low potential (−0.76 V vs. Standard hydrogen electrode (SHE)). To date, various ZIBs cathode materials with excellent performance have been developed, such as manganese- and vanadium-based oxides, Prussian blue and its analogues, and organic compounds. Unfortunately, some of these materials, especially manganese- and vanadium-based oxides, suffer from critical structural collapse, dissolution, and cathode/electrolyte interfacial side reactions, which lead to low Coulombic efficiency and poor cycle performance. The poor cycle performance is one of the main obstacles hindering the large-scale application of manganese- and vanadium-based oxides. Therefore, the structural design of cathodes and electrolyte regulation strategies have been extensively investigated to solve these problems and improve electrochemical performance. In comparison, electrolyte regulation is an important and effective strategy for improving the performance of ZIBs cathodes. It is well known that a strong interaction force exists between Zn²⁺ and H₂O, therefore, Zn²⁺ can coordinate with six H₂O molecules to form [Zn(H₂O)₆]²⁺ in the dilute aqueous electrolyte, while forming numerous hydrogen bonds between the H₂O molecules. The Zn²⁺-solvation structure and hydrogen bonds can be destructed and restructured by changing the anion, and using highly concentrated electrolyte and/or organic solvent, thereby decreasing the number of H₂O molecules in the solvated structure and the activity of free water. Furthermore, additives can change the pH value of the aqueous electrolyte and build a dissolution equilibrium between the cathode and electrolyte. Hence, an appropriate electrolyte regulation strategy can broaden the electrochemical stability window of electrolytes, improve the working potential, suppress the occurrence of interfacial side reactions, and prevent the dissolution of the active materials, thereby improving the electrochemical performance of ZIBs. Herein, we review the possible electrolyte regulation strategies for enhancing the electrochemical performance of ZIBs cathodes and classify regulation strategy into two main categories: 1) Solute (including different zinc salts, additive, and water-in-salt) and 2) Solvent (composite of organic/inorganic hybrid electrolytes). We then discuss the advantages and challenges of each strategy, and finally predict the possible future direction of electrolyte development.

Key words: Aqueous zinc-ion battery, Electrolyte, Cathode materials, Zn²⁺-solvation structure, Electrochemical performance

Yae Qi, Yongyao Xia. Electrolyte Regulation Strategies for Improving the Electrochemical Performance of Aqueous Zinc-Ion Battery Cathodes[J]. Acta Phys. -Chim. Sin. 2023, 39(2), 2205045. doi: 10.3866/PKU.WHXB202205045

Figures/Tables 14

Fig 1

Fig 2

Table 1

Fig 3

Fig 4

Fig 5

Fig 6

Fig 7

Fig 8

Fig 9

Table 2

The affection of solute regulation on electrochemical performance of cathode materials."

Type	Electrolytes	Cathodes	Potential window	Capacity/(mAh?g^?1)	Cycle performance	Ref.
Zinc salt	3 mol?L^?1 ZnSO₄	V⁵⁺-rich V₆O₁₃	0.2–1.4	520 at 0.5 A?g^?1	85% (1000/2 A?g^?1)	26
	3 mol?L^?1 Zn(CF₃SO₃)₂	(NH₄)_xV₂O₅?nH₂O	0.3–1.6	372 at 0.1 A?g^?1	80% (2000/5 A?g^?1)	49
	4 mol?L^?1 Zn(TFSI)₂	P(4VC₈₆-stat-SS₁₄)	0.25–2.0	324 at 1C	83% (48000/30C)	55
	1 mol?kg^?1 Zn(ClO₄)₂	VO₂	0.2–1.4	240 at 0.5 A?g^?1	500/2 A?g^?1	54
	1 mol?kg^?1 ZnCl₂	Ca_0.2V₂O₅?0.80H₂O	0.25–2.0	296 at 0.05 A?g^?1	8.4% (150/0.05 A?g^?1)	97
	0.5 mol?L^?1 Zn(CH₃COO)₂	Na₃V₂(PO₄)₃	0.8–1.7	97 at 0.05 A?g^?1	74% (100/0.05 A?g^?1)	106
Additives	1 mol?L^?1 ZnSO₄/1 mol?L^?1 Na₂SO₄	NaV₃O₈?1.5H₂O	0.3–1.25	380 at 0.1 A?g^?1	82% (1000/4 A?g^?1)	48
	0.5 mol?L^?1 ZnSO₄/0.25 mol?L^?1 K₂SO₄	ZnHCF	0.8–2.1	69.1 at 2C	74.1% (500/20C)	23
	3 mol?L^?1 ZnSO₄/0.5 mol?L^?1 Na₂SO₄	Na_0.56V₂O₅	0.4–1.5	317 at 0.1 A?g^?1	87% (1000/1 A?g^?1)	66
	1 mol?L^?1 ZnSO₄/1 mol?L^?1 MgSO₄	Mg_xV₂O₅?nH₂O	0.2–1.4	374 at 0.1 A?g^?1	90.3% (200/1 A?g^?1)	63
	2 mol?L^?1 ZnSO₄/0.2 mol?L^?1 CoSO₄	Co(III)rich-Co₃O₄	0.8–2.2	205 at 0.5 A?g^?1	92% (5000/4 A?g^?1)	73
	1 mol?L^?1 Zn(CF₃SO₃)₂/ 0.025 mol?L^?1 Zn(H₂PO₄)₂	V₂O₅	0.2–1.6	203 at 0.1 A?g^?1	88.1% (1000/0.8 A?g^?1)	77
	1 mol?L^?1 ZnSO₄/0.1 mol?L^?1 MnSO₄	ZnMn₂O₄	0.6–1.9	172 at 0.1 A?g^?1	79% (1000/2 A?g^?1)	107
	1 mol?L^?1 ZnSO₄/1 mol?L^?1 MnSO₄/ 0.1 mol?L^?1 H₂SO₄	MnO₂	0.8–2.2	570	92% (1800/0.03 A?cm^?2)	68
	1 mol?L^?1 ZnSO₄/1 mol?L^?1 urea (1 : 3)	Na_0.1MnO₂?0.5H₂O	1.0–1.8	270 at 0.1C	100 mAh?g^?1 (5000/10C)	76
	2 mol?L^?1 ZnSO₄/0.1 mol?L^?1 MnSO₄/ 0.5 mol?L^?1 Na₂SO₄	Na_0.55Mn₂O₄?1.5H₂O	0.8–1.9	367.5 at 0.65C	70% (10000/6.5C)	75
WiSE	21 mol?kg^?1 LiTFSI/1 mol?kg^?1 Zn(CF₃SO₃)₂	LiMn₂O₄	0.8–2.1	66 at 0.2C	80% (4000/4C)	80
	13 mol?kg^?1 ZnCl₂/0.8 mol?kg^?1 H₃PO₄	VOPO₄?xH₂O		170 at 0.1 A?g^?1	90 mAh?g^?1 (500/2 A?g^?1)	69
	1 mol?L^?1 HCl/20 mol?kg^?1 ZnCl₂	K₂NiFe(CN)₆	0.2–1.6	62.6 at 0.5 A?g^?1	76.1% (400/1 A?g^?1)	100
	30 mol?kg^?1 ZnCl₂	Ca_0.2V₂O₅?0.80H₂O	0.25–2.0	496 at 0.05 A?g^?1	51.1% (100/0.2C)	97
	30 mol?kg^?1 ZnCl₂	MoO₃	0.2–1.8	349 at 0.1 A?g^?1	73% (100/0.1 A?g^?1)	102
	15 mol?kg^?1 NaClO₄/1 mol?kg^?1 Zn(CF₃SO₃)₂	C-NaVPO₄F	0.6–1.8	87.4 at 0.1 A?g^?1	89.3% (4000/1 A?g^?1)	98
	2 mol?L^?1 Zn(OTf)₂/8 mol?kg^?1 LiOTf	VO₂	0.3–1.3	260 at 0.1 A?g^?1	89.7% (10000/10 A?g^?1)	85
	67% (w) Malt /2 mol?kg^?1 ZnSO₄	NH₄V₄O₁₀	0.4–1.4	400 at 0.05 A?g^?1	100% (4000 /5A?g^?1)	103

Table 2

Fig 10

Fig 11

Table 3

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Electrolyte	Ionic conductivity/(mS?cm^?1)	pH	Cost	Feature and function	Ref.
2 mol?L^?1 ZnSO₄	56.9	4.9	Low	High stability, the most common electrolyte	54
2 mol?L^?1 Zn(CF₃SO₃)₂	58.6 ³⁸	3.6	High	Large volume, high capacity and fast reaction kinetics	49
4 mol?L^?1 Zn(TFSI)₂	90	3.5	High	Weak solvation，can suppress side reaction and improve coulombic efficiency	55
2 mol?kg^?1 ZnCl₂	84.2	4.2	High	Low decomposition voltage, high solubility, common WiSE	45
2 mol?kg^?1 Zn(CH₃COO)₂	10.9 ³⁸	5.7	Low	pH near neutral, friendly to Zn electrode	54
2 mol?kg^?1 Zn(NO₃)₂	115.6 ³⁸		Low	NO₃^? processes strong oxidation	47
1 mol?kg^?1 Zn(ClO₄)₂	48	4.9	Low	Chaotropic salt, excellent electrochemical performance at low-temperature	52, 53

Organic agent	(H₂O : organic)	Roles	Freezing point (℃)	Boiling point (℃)	Flash point (℃)	Dielectric constant	Viscosity (mPa?s)	Ref.
ACN	3 : 1	Shielding free water, building stable phase interface and suppressing HER and Zn dendrites.	?45.7	81.6	5.6	37.5	0.441	106
DMSO	4.3 : 1	Reconstruct Zn²⁺-sheath, forming SEI in situ, inhibiting decomposition of H₂O.	19	189	89	47.2	1.996	107
Diethyl ether	98 : 2	Acting electrostatic shield layer, leading to uniform deposition.	?116.2	34.5	?45	4.2	0.233	109
Methyl alcohol	1 : 1	Reducing water activity, weaken Zn²⁺ solvation structure.	?98	64.8	11	33	0.545	110
Ethyl alcohol	5 : 95	Suppressing dissolution of cathode, Zn dendrite and HER.	?114	78.3	21	25.7	1.074	114
Ethylene glycol	3 : 2	Hydrogen bonding of EG-H₂O, excellent performance at low temperature	?12.9	197.3	111	37	16.1	103
Glycerol	1 : 1	Glycerol has strong binding interaction with Zn metal, take part in Zn²⁺ solvation sheath structure.	18.2	290	177	19.9	800	112
DME	3 : 2	Forming organic/inorganic hybrid ZnF₂-ZnS-rich interphase in situ.	?58	85	?2	5.5		115
TEP	1 : 1	Occupying Zn²⁺-solvation sheath, SEI in situ.	?56.5	215	117	13.2	1.46	38
PC	4 : 1	Have a good stability at high voltage	?48.8	242	132	65	1.2	118

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Electrolyte Regulation Strategies for Improving the Electrochemical Performance of Aqueous Zinc-Ion Battery Cathodes

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