钠离子电池钒基聚阴离子型正极材料的发展现状与应用挑战

doi:10.19799/j.cnki.2095-4239.2020.0179

储能科学与技术 ›› 2020, Vol. 9 ›› Issue (5): 1350-1369.doi: 10.19799/j.cnki.2095-4239.2020.0179

钠离子电池钒基聚阴离子型正极材料的发展现状与应用挑战

易红明^1,²(), 吕志强^1,², 张华民¹, 宋明明³, 郑　琼¹(), 李先锋¹()

^1.中国科学院大连化学物理研究所，辽宁大连 116023
^2.中国科学院大学，北京 100039
^3.大连博融新材料有限公司，辽宁大连 116023

收稿日期:2020-05-17 修回日期:2020-05-28 出版日期:2020-09-05 发布日期:2020-09-08
通讯作者: 郑　琼,李先锋 E-mail:yihm@dicp.ac.cn;zhengqiong@dicp.ac.cn;lixianfeng@dicp.ac.cn
作者简介:易红明（1993—），男，博士，研究方向为钠离子电池，E-mail：yihm@dicp.ac.cn；
基金资助:
中国科学院洁净能源创新研究院合作基金项目(DNL2019);中国科学院A类战略性先导科技专项课题(XDA21070500)

Recent progress and application challenges in V-based polyanionic compounds for cathodes of sodium-ion batteries

Hongming YI^1,²(), Zhiqiang LYU^1,², Huamin ZHANG¹, Mingming SONG³, Qiong ZHENG¹(), Xianfeng LI¹()

^1.Dalian Institute of Chemical Physics, Dalian 116023, Liaoning, China
^2.University of Chinese Academy of Sciences, Beijing 100039, China
^3.Dalian Bolong New Materials Co. Ltd. , Dalian 116023, Liaoning, China

Received:2020-05-17 Revised:2020-05-28 Online:2020-09-05 Published:2020-09-08
Contact: Qiong ZHENG,Xianfeng LI E-mail:yihm@dicp.ac.cn;zhengqiong@dicp.ac.cn;lixianfeng@dicp.ac.cn

摘要/Abstract

摘要：

钠离子电池以其资源丰富、性价比高等优势有望在电动自行车、低速电动车、固定式储能领域获得广泛应用。在众多正极材料中，钒基聚阴离子型化合物因具有能量密度高、功率密度高、稳定性好等优点成为研究热点之一。但是其本征电子电导率较低，同时由于制备方法不当等带来的体相电子和离子传递阻力较大等缺陷，限制了材料的实际比容量、倍率性能及稳定性等。本文从几种典型的钒基聚阴离子型化合物的晶胞结构和储钠特性分析入手，从微观材料本体和介观电极结构的角度讨论钒基聚阴离子型化合物中电荷传递过程、动力学提升策略并总结近期进展；结合钒基聚阴离子型化合物的实用化需求，凝练出推进钒基聚阴离子型化合物进一步发展的重要研究方向。

关键词: 钠离子电池, 正极材料, 钒基聚阴离子型化合物, 电荷传递动力学, 低成本规模化制备, 实用化

Abstract:

Sodium-ion batteries have potential applications in the field of electric bicycles, low-speed electric vehicles, and stationary energy storage due to the abundance and low cost of sodium resources. Of the various cathode materials proposed for sodium-ion batteries, vanadium (V)-based polyanionic compounds have become a research hotpot due to their high energy density, high power density, and stable structure. However, the low intrinsic conductivity and improper preparation method of such compounds impede their bulk electron and ion transfer, which limit the specific capacity, rate capability, and structure stability of these materials. In this review, starting from an analysis of the cell structure and sodium storage characteristics of several typical V-based polyanionic compounds, we review the charge transfer process, strategy for improving the kinetics, and progress in V-based polyanionic compounds from the perspective of the microstructure and mesoscopic electrode structure. Meanwhile, combined with a discussion of the practical applications of V-based polyanionic compounds, the important research directions to promote the further development of V-based polyanionic compounds are summarized.

Key words: sodium-ion batteries, cathode materials, V-based polyanionic compounds, charge transfer kinetics, low-cost and scale preparation, industrialization

中图分类号:

TQ 028.8

易红明, 吕志强, 张华民, 宋明明, 郑　琼, 李先锋. 钠离子电池钒基聚阴离子型正极材料的发展现状与应用挑战[J]. 储能科学与技术, 2020, 9(5): 1350-1369.

Hongming YI, Zhiqiang LYU, Huamin ZHANG, Mingming SONG, Qiong ZHENG, Xianfeng LI. Recent progress and application challenges in V-based polyanionic compounds for cathodes of sodium-ion batteries[J]. Energy Storage Science and Technology, 2020, 9(5): 1350-1369.

图/表 15

图1

表1

典型的钒基聚阴离子型化合物的主要特征参数和性能水平"

材料体系	材料名称	晶体结构类型	氧化还原电对	氧化还原电位/V	理论比容量/mA·h·g^-1	理论能量密度 /W·h·kg^-1	储钠机理	钠扩散系数 /cm·s^-1	电化学性能
正磷酸盐	Na₃V₂(PO₄)₃^[11]	rhombohedral (NASICON, $R 3 ˉ c$ )	V⁴⁺/V³⁺	3.4	117.6	400	bi-phase reaction	1.06×10^-11 /CV	107.1 mA·h/g at 0.1 C
	Na₃V₂(PO₄)₃^[12]	rhombohedral (NASICON, $R 3 ˉ c$ )	V⁴⁺/V³⁺	3.4	117.6	400	bi-phase reaction	9.6×10^-11 /CV	117 mA·h/g at 1 C 82 mA·h/g at 100 C
	NaVOPO₄^[13]	monoclinic	V⁵⁺/V⁴⁺	3.6	145	522	single-phase reaction	1-3×10^–11 /GITT	101 mA·h/g at 5 C
	NaVOPO₄^[14]	orthorhombic	V⁵⁺/V⁴⁺	3.3	145	479	—	—	115 mA·h/g at 0.1 C
	KVOPO₄^[15]	orthorhombic	V⁵⁺/V³⁺	2.56	266.7	683		9.6 × 10^-12 /CV	235 mA·h/g at 0.05 C
	NaVOPO₄^[16]	tetragonal (layered structure)	—	—	—	—	—	—	—
	NaVOPO₄^[17]	triclinic	V⁵⁺/V⁴⁺	3.5	145	508	multi-phase reactions	4.9 × 10^-11 /EIS	144 mA·h/g at 0.05 C 58 mA·h/g at 5 C
	VOPO₄^[18]	tetragonal (layered structure)	V⁵⁺/V⁴⁺	3.4	165.5	563	—	—	150 mA·h/g at 0.05 C
	Na₃V₃(PO₄)₄^[19]	monoclinic (layered structure, C2/c)	V⁴⁺/V³⁺	3.9	44.5	174	—	—	>40 mA·h/g at 0.6 C 36.9 mA·h/g at 3 C
	Na₃V(PO₄)₂^[20]	monoclinic (layered structure, C2/c)	V⁴⁺/V³⁺	3.5	90	315	—	—	>90 mA·h/g at 0.2 C 71 mA·h/g at 15 C
	Na₄VO(PO₄)₂^[21]	orthorhombic (Pbca)	V⁵⁺/V⁴⁺	3.5	78	273	single-phase reaction	—	41.3 mA·h/g at 10 C
氟磷酸盐	NaVPO₄F^[22]	tetragonal (NASICON, I4/mmm)	V⁴⁺/V³⁺	3.7	142.5	485	—	—	120.9 mA·h/g at 0.05 C 70.1 mA·h/g at 0.5 C
	NaVPO₄F^[23]	monoclinic (NASICON, C2/c)	V⁴⁺/V³⁺	3.4	142.5	484.5	single-phase reaction	—	135 mA·h/g at 0.2 C 112 mA·h/g at 30 C
	Na₃V₂(PO₄)₂F₃^[24,25]	tetragonal (NASICON, P4₂/mnm)	V⁴⁺/V³⁺	3.9	128.3	500	bi-phase reaction and single-phase reaction	10^-12 /EIS	125 mA·h/g at 0.2 C 104 mA·h/g at 40 C 41 mA·h/g at 200 C
	Na₃V₂(PO₄)₂O₂F^[10,26]	tetragonal (I4/mmm)	V⁵⁺/V⁴⁺	3.8	130	494	two completely reversible bi-phasic reaction	—	127.4 mA·h/g at 0.2 C 84.1 mA·h/g at 40 C
	Na₃V₂(PO₄)₂O_1.6F_1.4^[27]	tetragonal (P4₂/mnm)	V⁵⁺/V^3.8+	3.8	155.6	592	single-phase reaction	2.4×10^-12 /EIS	134 mA·h/g at 0.1 C
焦磷酸盐	Na₇V₃(P₂O₇)₄^[28]	monoclinic (C2/c)	V⁴⁺/V³⁺	4.13	79.6	329	single-phase reaction	—	67.2 mA·h/g at 8 C
	Na₂(VO)P₂O₇^[29]	tetragonal (P21/c)	V⁵⁺/V⁴⁺	3.8	93.4	355	—	—	80 mA·h/g at 0.05 C
	NaVP₂O₇^[30]	monoclinic	V⁴⁺/V³⁺	3.9	108.1	421	—	—	104 mA·h/g at 0.1 C
混合聚阴离子型	Na₇V₄(P₂O₇)₄(PO₄)^[31]	tetragonal (P $4 ˉ$ 21c)	V⁴⁺/V³⁺	3.85	92.7	357	bi-phasic reaction	—	92 mA·h/g at 0.05 C 70.2 mA·h/g at 10 C

表1

图2

图3

图4

图5

图6

图7

图8

图9

图10

图11

图12

图13

图14

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钠离子电池钒基聚阴离子型正极材料的发展现状与应用挑战

Recent progress and application challenges in V-based polyanionic compounds for cathodes of sodium-ion batteries

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