Research Progress of LiTi2(PO4)3 Anode for Aqueous Lithium-ion Batteries

doi:10.15541/jim20210502

Abstract

Abstract:

As green rechargeable batteries, lithium-ion batteries feature high energy and power density. However, commonly-used electrolytes, organic compounds, in commercially available lithium-ion batteries are flammable and toxic, which leaves them at the risk of combustion and explosion when being overcharged or short-circuited. In order to solve this problem, much attention has been paid to lithium-ion batteries with aqueous electrolytes, which take low-toxicity and high safety as the prominent advantages. The working voltage, 1.5-2.0 V, indicates their usage mainly in the field of energy storage. Considering the hydrogen and oxygen evolution, conventional anode materials used in commercially available lithium-ion batteries are inconformity for water-based lithium-ion batteries. Therefore, the key to the development of aqueous lithium-ion batteries lies in the selection of anodes. The anode material, LiTi₂(PO₄)₃, has drawn the attention of researchers due to its advantages such as three-dimensional channel, and appropriate lithium-ion intercalation potential. The synthesis methods of LiTi₂(PO₄)₃ mainly include high temperature solid-phase calcination, Sol-Gel methods and hydrothermal reaction, etc. To further improve the electrochemical performance of LiTi₂(PO₄)₃, strategies can be used such as particle nanocrystallization, morphology control, element doping, and carbon-coating, etc. This review focuses on the synthesis and modification of LiTi₂(PO₄)₃, as well as related research progress. At last, the future development of LiTi₂(PO₄)₃ as anode material for lithium-ion battery is properly prospected.

Key words: aqueous lithium-ion battery, anode material, LiTi₂(PO₄)₃, review

CLC Number:

TM912

WANG Yutong, ZHANG Feifan, XU Naicai, WANG Chunxia, CUI Lishan, HUANG Guoyong. Research Progress of LiTi₂(PO₄)₃ Anode for Aqueous Lithium-ion Batteries[J]. Journal of Inorganic Materials, 2022, 37(5): 481-492.

Figures/Tables 10

References 93

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Type	Operating voltage/V	Safety	Electrolyte	Solvent	Cost
Organic Li-ion battery	3.6-4.2	Low	LiPF₆, LiAsF₆, etc	EC, DMC, DEC, etc	High
Aqeuous Li-ion battery	1.5-2.0	High	Li₂SO₄, LiNO₃, etc	H₂O	Moderate

Type	Operating voltage/V	Safety	Electrolyte	Solvent	Cost
Organic Li-ion battery	3.6-4.2	Low	LiPF₆, LiAsF₆, etc	EC, DMC, DEC, etc	High
Aqeuous Li-ion battery	1.5-2.0	High	Li₂SO₄, LiNO₃, etc	H₂O	Moderate

Anode material	Specific capacity/ (mAh·g^-1)	Potential/ V(vs. Li⁺/Li)	Potential/ V(vs. NHE)	Features
LiTi₂(PO₄)₃	138	2.5	-0.5	Moderate specific capacity, stable framework
TiP₂O₇	121	2.6	-0.4	Low specific capacity, high Li-intercalation potential
VO₂	250	2.6	-0.4	High specific capacity, poor cycling performance
LiV₃O₈	250	2.6	-0.4	Fragile during cycling

Anode material	Specific capacity/ (mAh·g^-1)	Potential/ V(vs. Li⁺/Li)	Potential/ V(vs. NHE)	Features
LiTi₂(PO₄)₃	138	2.5	-0.5	Moderate specific capacity, stable framework
TiP₂O₇	121	2.6	-0.4	Low specific capacity, high Li-intercalation potential
VO₂	250	2.6	-0.4	High specific capacity, poor cycling performance
LiV₃O₈	250	2.6	-0.4	Fragile during cycling

Method	Starting materials			Product characteristic	Features	Ref.
	Li source	Ti source	P source	Morphology	Features	Ref.
Solid state	LiH₂PO₄	TiO₂	NH₄H₂PO₄	Irregular particles	Long calcination time, high temperature	[20]
Sol-Gel	CH₃COOLi	Ti(C₄H₉O)₄	H₃PO₄	Particles	Short calcination time, low temperature	[21]
Hydrothermal synthesis	CH₃COOLi	Ti(C₄H₉O)₄	NH₄H₂PO₄	Regular particles	Regular particle morphology, great crystallinity	[22]
Co-precipitation method	LiOH	Ti(C₄H₉O)₄	H₃PO₄	Particles	Requiring precise control	[23]
Electrospinning	CH₃COOLi	Ti(C₄H₉O)₄	NH₄H₂PO₄	Fiber	Ideal electrochemical performance, difficult industrialization	[24]

Research Progress of LiTi₂(PO₄)₃ Anode for Aqueous Lithium-ion Batteries

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Calcination parameter	Coating method	Carbon source	Weight percentage of carbon/%	Current density/(mA·g^-1)	Specific capacity (cycles)/(mAh·g^-1)	Capacity retention/%	Ref.
800 ℃-12 h	In-situ	Citric acid	6.2	138	106.1(1)-89(1300)	84	[36]
900 ℃-12 h	Ex-situ	Toluene	12	700	100(1)-83(200)	83	[31]
800 ℃-12 h	Ex-situ	Acetylene Black	18	140	106.3(1)-86.5(100)	81	[81]
850 ℃-12 h	Ex-situ	Acetylene Black	-	1400	91.3(1)-74.4(100)	81	[82]
700 ℃-12 h	In-situ	Pitch	17.5	1380	107(1)-75.5(1000)	70	[83]
550 ℃-24 h	In-situ	Sucrose	3.5	1400	110(1)-104(800)	94	[17]
750 ℃-5 h	In-situ	Polyaniline	5.9	276	115.2(1)-94.6(1000)	82	[84]
750 ℃-5 h	In-situ	Polyacrylonitrile	5.9	690	95(1)-82.1(1000)	86	[85]
900 ℃-12 h	In-situ	Graphene oxide	1.79	~1380	110(1)-100(100)	91	[78]
800 ℃-10 h	In-situ	Graphene oxide	-	~276	105(1)-97.86(100)	93.2	[77]
700 ℃-5 h	In-situ	Graphene oxide, phenolic resin	16.2	~690	101.1(1)-78(1000)	77.2	[80]
800 ℃-8 h	Ex-situ	β-Cyclodextrin	3.13	~690	120(1)-(200)111.3	88.7	[86]

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