水系锂离子电池负极材料LiTi2(PO4)3的研究进展

doi:10.15541/jim20210502

无机材料学报 ›› 2022, Vol. 37 ›› Issue (5): 481-492.DOI: 10.15541/jim20210502 CSTR: 32189.14.10.15541/jim20210502

所属专题：【能源环境】锂离子电池(202409)

水系锂离子电池负极材料LiTi₂(PO₄)₃的研究进展

王禹桐¹(), 张非凡¹, 许乃才², 王春霞¹, 崔立山¹, 黄国勇¹()

1. 中国石油大学(北京) 新能源与材料学院, 重质油国家重点实验室, 北京 102249
2. 青海师范大学化学化工学院, 西宁 810008

收稿日期:2021-08-13 修回日期:2021-10-22 出版日期:2022-05-20 网络出版日期:2021-11-01
通讯作者: 黄国勇, 教授. E-mail: huanggy@cup.edu.cn
作者简介:王禹桐(1992-), 男, 博士研究生. E-mail: 1248736790@qq.com;
基金资助:
国家自然科学基金(52022109);国家自然科学基金(51834008);北京市自然科学基金(2202047);中国石油大学(北京)科研基金(2462018YJRC041);中国石油大学(北京)科研基金(2462020YXZZ016)

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

WANG Yutong¹(), ZHANG Feifan¹, XU Naicai², WANG Chunxia¹, CUI Lishan¹, HUANG Guoyong¹()

1. State Key Laboratory of Heavy Oil, College of New Energy and Materials, China University of Petroleum-Beijing, Beijing 102249, China
2. School of Chemistry and Chemical Engineering, Qinghai Normal University, Xining 810008, China

Received:2021-08-13 Revised:2021-10-22 Published:2022-05-20 Online:2021-11-01
Contact: HUANG Guoyong, professor. E-mail:huanggy@cup.edu.cn
About author:WANG Yutong (1992-), male, PhD candidate. E-mail: 1248736790@qq.com
Supported by:
National Natural Science Foundation of China(52022109);National Natural Science Foundation of China(51834008);Beijing Municipal Natural Science Foundation(2202047);Science Foundation of China University of Petroleum, Beijing(2462018YJRC041);Science Foundation of China University of Petroleum, Beijing(2462020YXZZ016)

摘要/Abstract

摘要：

锂离子电池作为一种绿色可充电电池, 具有较高的能量密度及功率密度, 但市售锂离子电池主要以有机物为电解液, 当电池过充或短路时存在一定的燃烧及爆炸风险。为应对此问题, 水系锂离子电池逐渐走进人们的视野, 它具有清洁环保、安全性能高等优点, 其工作电压为1.5~2.0 V, 主要应用于储能领域。考虑到水系电池的析氢析氧反应, 常规负极材料无法应用于水系锂离子电池, 因此水系锂离子电池的研发关键在于负极材料的选取。LiTi₂(PO₄)₃具有开放的三维通道以及合适的嵌锂电位, 可以作为水系锂离子电池的负极材料。LiTi₂(PO₄)₃的合成方法主要有高温固相法、溶胶-凝胶法和水热法等。为进一步提高LiTi₂(PO₄)₃的电化学性能, 可以采用颗粒纳米化、形貌控制、元素掺杂及碳包覆等方式进行改性。本文从合成方法及改性手段的角度, 对近年来国内外水系锂离子电池负极材料LiTi₂(PO₄)₃的研究进行综述, 并对LiTi₂(PO₄)₃负极材料的发展前景做出展望。

关键词: 水系锂离子电池, 负极材料, LiTi₂(PO₄)₃, 综述

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

中图分类号:

TM912

王禹桐, 张非凡, 许乃才, 王春霞, 崔立山, 黄国勇. 水系锂离子电池负极材料LiTi₂(PO₄)₃的研究进展[J]. 无机材料学报, 2022, 37(5): 481-492.

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.

图/表 10

表1 水系锂离子电池和有机系锂离子电池的特征比较[8]

Table 1 Comparison of the characteristics of aqeuous and organic lithium-ion batteries[8]

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

图1 电极材料的嵌锂电位-pH的关系图

Fig. 1 Potential-pH diagram of typical electrode materials

表2 部分水系锂离子电池的负极材料的参数[14]

Table 2 Parameters of some anode materials for aqeuous lithium-ion battery[14]

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

图2 LiTi2(PO4)3的晶体结构图[17]

Fig. 2 Crystal structure of LiTi2(PO4)3[17]

表3 常见LiTi2(PO4)3合成方法比较

Table 3 Comparison of common synthetic methods of LiTi2(PO4)3

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]

图3 LiTi2(PO4)3 纳米线(LTPNMs)的制备过程示意图[38]

Fig. 3 Schematical illustration of the fabrication process of lithium titranium phosphate nanowires (LTPNMs)[38]

图4 静电纺丝法示意图(a), LiTi2(PO4)3纤维与颗粒的倍率性能曲线(b)[24]

Fig. 4 Schematic diagram of electrospinning (a), comparison of rate performance between LiTi2(PO4)3 fibers and particles (b)[24]

图5 四种包覆碳源的倍率性能图 (a, b)[72]((a)蓝、黑分别为聚多巴胺和酚醛树脂; (b)蓝、黑分别为聚丙烯腈和葡萄糖), 具有均质碳层的介孔LiTi2(PO4)3中Li+插入的机制示意图(c)[75], rGO-LTP的合成步骤示意图(d)[78], LC和LCG在5C下循环1000次的循环性能曲线(e)[80]

Fig. 5 Comparison chart of rate performance of four coated carbon sources (a, b)[72](Blue and black in (a) indicating polydopamine and phenolic resin; blue and black in (b) indicating polyacrylonitrile and glucose), schematic illustration of the tentative Li+ insertion mechanism in mesoporous LiTi2(PO4)3 with carbon coating layer (c)[75], schematic diagram of the synthesis steps of rGO-LTP (d)[78], and cyclic performance of LC and LCG anodes at 5C for 1000 cycles (e)[80] Colorful figures are available on website

表4 溶胶-凝胶法不同碳源和包覆方式的电性能比较

Table 4 Comparison of electrochemical performance of different carbon sources and coating methods by Sol-Gel

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]

图6 LiTi2(PO4)3/C和LiTi1.8Sn0.2(PO4)3/C在不同电流密度下连续循环的放电容量(a), 电流密度为4和6 A·g-1时的长期循环性能(b)[24]

Fig. 6 Discharge capacity for successive cycling at different current densities (a), long-term cycling behavior at current densities of 4 and 6 A·g-1 (b) of LiTi2(PO4)3/C and LiTi1.8Sn0.2(PO4)3/C[24]

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水系锂离子电池负极材料LiTi₂(PO₄)₃的研究进展

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

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