聚阴离子型钠离子电池正极材料的研究进展

doi:10.3866/PKU.WHXB201905017

物理化学学报 >> 2020, Vol. 36 >> Issue (5): 1905017.doi: 10.3866/PKU.WHXB201905017

所属专题：钠离子储能材料和器件

聚阴离子型钠离子电池正极材料的研究进展

潘雯丽,关文浩,姜银珠*()

浙江大学材料科学与工程学院，硅材料国家重点实验室，杭州 310027

收稿日期:2019-05-02 录用日期:2019-06-18 发布日期:2019-06-24
通讯作者: 姜银珠 E-mail:yzjiang@zju.edu.cn
作者简介:姜银珠，浙江大学教授，1983年出生。1998–2007年在中国科学技术大学本硕博学习，2007–2010年分别在亚申科技研发中心、英国Heriot-Watt大学、德国Bielefeld大学从事研究工作，2010年起加入浙江大学。主要从事电化学储能材料与器件研究
基金资助:
国家自然科学基金(51722105);浙江省自然科学基金(LR18B030001);中央高校基本科研业务费(2018XZZX002-08)

Research Advances in Polyanion-Type Cathodes for Sodium-Ion Batteries

Wenli Pan,Wenhao Guan,Yinzhu Jiang*()

State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, P. R. China

Received:2019-05-02 Accepted:2019-06-18 Published:2019-06-24
Contact: Yinzhu Jiang E-mail:yzjiang@zju.edu.cn
Supported by:
the National Natural Science Foundation of China(51722105);the Zhejiang Provincial Natural Science Foundation, China(LR18B030001);the Fundamental Research Funds for the Central Universities, China(2018XZZX002-08)

摘要/Abstract

摘要：

作为钠离子电池正极材料的体系之一，聚阴离子型化合物具有成本低廉和安全性高的优点，适合于大规模固定式储能系统。实时平衡电网电力供需水平对正极材料的倍率性能提出了更高的要求，而聚阴离子材料虽然存在离子扩散通道，但缺乏电子传输路径，导致其动力学性能不佳。为了挖掘影响聚阴离子型正极动力学性能的因素，本文以结构为基础，对影响聚阴离子正极离子扩散行为的本征原因作了阐述，再从表面修饰和形态设计入手，对目前研究较多的改善电极表面及界面处离子和电子扩散的策略作了总结与点评，然后从材料的分级结构回归到鲜见报导的元素掺杂和取代，从本质上提出优化动力学性能的方案，并展望了进一步提高正极材料倍率性能的方向。本文可为高倍率的聚阴离子型正极材料及其他材料的开发提供基本理论和实践依据。

关键词: 钠离子电池, 聚阴离子型正极, 高倍率性能, 离子扩散, 电子传输

Abstract:

Because of their high energy density and long cycle life, lithium-ion batteries (LIBs) have dominated the portable electronics market for over 20 years. However, with the increasing demand for large-scale energy storage systems for grid applications, the price of Li resources has increased owing to the low abundance of Li in Earth's crust and non-uniform distribution on the planet. Because Na has similar physical and chemical properties as Li and is an abundant natural resource, room-temperature sodium-ion batteries (SIBs) are expected to be among the most promising next-generation large grid energy storage devices. It is known that the cathode, anode, separator and electrolyte materials are the main components of batteries. Among these, Na-containing cathode materials are of critical importance. As a cathode material for SIBs, polyanion-type compounds have become a hot research topic owing to their versatile structural frameworks, high thermal stabilities, high ambient stabilities even in the charging state, small volume changes, tunable operating voltage by tuning the chemical environment of the polyanions, and high operating voltages owing to the inductive effects of the polyanionic groups (PO₄³⁻, SO₄²⁻, SiO₄⁴⁻, etc.). In particular, for Earth's abundant resources and inherent stability, polyanion-based compounds are suitable for large-scale stationary energy storage. Taking grid balancing into account, batteries with fast charge rates are in demand, which requires cathodes having high rate capability. However, despite the presence of ion diffusion channels in polyanion compounds, the electronic transport channels are blocked owing to the separation of the metal polyhedral and the strong electronegativity of the anions, leading to poor electron conductivity, which largely limits the rate capability of polyanion compounds. Therefore, it is crucial to understand the inherent limitation of the kinetics in terms of the structural aspects and to determine strategies for improving the rate capability. This review discusses the intrinsic reasons for the factors impacting ion diffusion based on the different structures of polyanion-type cathodes. From the perspectives of surface modification and morphology, strategies for enhancing the transport of sodium ions and electrons at the surface and interface are summarized and discussed. Then, from the standpoint of the hierarchical structures of materials to the design of a structural framework, which have been rarely reported, this review proposes schemes that intrinsically enhance the rate capability of polyanion compounds and provides a perspective on developments that can further improve the rate capability of cathode materials. This review provides suggestions for designing and optimizing high-rate polyanion-type and other kinds of cathodes from both academic and practical viewpoints.

Key words: Sodium-ion battery, Polyanion-type cathode, High rate capability, Ion diffusion, Electron transport

潘雯丽,关文浩,姜银珠. 聚阴离子型钠离子电池正极材料的研究进展[J]. 物理化学学报, 2020, 36(5), 1905017. doi: 10.3866/PKU.WHXB201905017

Wenli Pan,Wenhao Guan,Yinzhu Jiang. Research Advances in Polyanion-Type Cathodes for Sodium-Ion Batteries[J]. Acta Physico-Chimica Sinica 2020, 36(5), 1905017. doi: 10.3866/PKU.WHXB201905017

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201905017

https://www.whxb.pku.edu.cn/CN/Y2020/V36/I5/1905017

图/表 10

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表1

表2

不同聚阴离子钠电正极材料的倍率性能"

Chemical formula	Theoretical Capacity/(mAh?g^?1)	Materials and ways to improve rate performance	Electrochemical data	Ref.
Maricite-NaFePO₄	150	Nano-NaFePO₄ (50 nm)/C	142 mAh?g^?1 at C/20 and 60 mAh?g^?1 at 2C	20
		Nano-NaFePO₄ (40–140 nm)/C/graphene	142 mAh?g^?1 at C/20 and 51 mAh?g^?1 at 5C	62
		Nano-NaFePO₄ (1.6 nm) @ porous N-doped carbon nanofibers	145 mAh?g^?1 at 0.2C and 61 mAh?g^?1 at 50C	53
Oviline-NaFePO₄	150	Bare NaFePO₄	125 mAh?g^?1 at 7.5 mA?g^?1	17
Oviline-NaFePO₄	150	Polythiophene-Wrapped NaFePO₄	141 mAh?g^?1 at 10 mA?g^?1 and 42 mAh?g^?1 at 300 mA?g^?1	64
Na₂FeP₂O₇	97	Na₂FeP₂O₇ (300-500 nm)/C	82 mAh?g^?1 at C/20 and 50 mAh?g^?1 at 10C	65
Na₂FeP₂O₇	97	Na₂FeP₂O₇/MWCNT	86 mAh?g^?1 at 1C and 68 mAh?g^?1 at 10C	57
Na₃V₂(PO₄)₃	118	Na₃V₂(PO₄)₃/C	93 mAh?g^?1 at C/20 and 29 mAh?g^?1 at 1C	66
		Na₃V₂(PO₄)₃ (20-40 nm) @ Porous Carbon Matrix	102 mAh?g^?1 at 20C and 44 mAh?g^?1 at 200C	28
		Na₃V₂(PO₄)₃ (50-200 nm) @C@rGO	115 mAh?g^?1 at 20C and 86 mAh?g^?1 at 100C	67
Na₃V₂(PO₄)₂F₃	128	Core/double-shell structured Na₃V₂(PO₄)₂F₃@C	120 mAh?g^?1 at 1C and 63 mAh?g^?1 at 100C	68
Na₃(VO)₂(PO₄)₂F	130	Na₃(VO)₂(PO₄)₂F /C	102 mAh?g^?1 at 20C and 68 mAh?g^?1 at 1C	69
Na₃(VO)₂(PO₄)₂F	130	Graphene quantum dots-shielded Na₃(VO)₂(PO₄)₂F @C nanocuboids	102 mAh?g^?1 at 20C and 70 mAh?g^?1 at 45C	60
Na₂Fe(SO₄)₂· 2H₂O	82	Bare- Na₂Fe(SO₄)₂·2H₂O	70 mAh?g^?1 at C/20	42
Na₂Fe(SO₄)₂· 2H₂O	82	Na₂Fe(SO₄)₂·2H₂O@ zero-, one and two-dimensional carbon matrix (activated carbon, single wall carbon nanotubes and graphene)	60 mAh?g^?1 at 5C	44
Na_2+2xFe_2-x(SO₄)₃ (x = 0–0.4)	120	Bare Na_2+2xFe_2?x(SO₄)₃	102 mAh?g^?1 at C/20 and 58 mAh?g^?1 at 20C	49
Na_2+2xFe_2-x(SO₄)₃ (x = 0–0.4)	120	Na_2+2xFe_2?x(SO₄)₃/SWNT	60 mAh?g^?1 at 40C	51
Na₂FeSiO₄	276	Na₂FeSiO₄ (30–50 nm)/C	106 mAh?g^?1 at 10 mA?g^?1 and 40 mAh?g^?1 at 200 mA?g^?1	34
		Na₂FeSiO₄ (20–50 nm)/C	106 mAh?g^?1 at 27.6 mA g^?1 (0.1C) and 100 mAh?g^?1 at 276 mA?g^?1 (1C)	35
		mesoporous Na₂FeSiO₄ nanospheres @ carbon nanotubes	173 mAh?g^?1 at 0.1C and 109 mAh?g^?1 at 20C	70
Na₂MnSiO₄	280	Na₂MnSiO₄ with 5% (volume percent) VC electrolyte additive	210 mAh?g^?1 at 0.1C and 100 mAh?g^?1 at 5C	37
Na₂MnSiO₄	280	three-dimensionally ordered macroporous Na₂MnSiO₄/C	207 mAh?g^?1 at 0.1C and 76 mAh?g^?1 at 5C	38

表2

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图8

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聚阴离子型钠离子电池正极材料的研究进展

Research Advances in Polyanion-Type Cathodes for Sodium-Ion Batteries

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	Chemical formula	Space group	Dimensions of ion channels	Sodium diffusion coefficient/(cm²·s^?1)	Ref.
Phosphates	Maricite-NaFePO₄	Pnma	none	4.79 × 10^?11 (nano amorphous particles)	20
	Olivine-NaFePO₄	Pnma	one	8.63 × 10^?17	18
	Na₂FeP₂O₇	P${\rm{\bar 1}}$	three	(2.79–8.45) × 10^?13	57
	Na₂CoP₂O₇	P${\rm{\bar 1}}$	three	/	23
		P21cn	two	/	23
		P42/mnm	three	/	23
	Na₃V₂(PO₄)₃	R${\rm{\bar 3}}$cH	three	4.59 × 10^?13–2.45 × 10^?10	58
	Na₃V₂(PO₄)₂F₃	P42/mnm	three	2.68 × 10^?12	59
	Na₃(VO)₂(PO₄)₂F	P42/mnm	three	(1–3) × 10^?10	60
Sulfates	Na₂Fe(SO₄)₂·2H₂O	P21/c	two	10^?14	44
	Na₂Fe(SO₄)₂·4H₂O	P21/c	one	/	45
	NaFe(SO₄)₂	C12/m1	two	9.01 × 10^?10 (1273 K)	47
	Na_2+2xFe_2?x(SO₄)₃	P21/c	three	1 × 10^?7	61
Orthosilicate	Na₂FeSiO₄	P${\rm{\bar 1}}$	three	(1.92–2.53) × 10^?13	35
	Na₂MnSiO₄	Pn	one	2.37 × 10^?15–8.62 × 10^?14	38
	Na₂CoSiO₄	Pn2a	Three	1.29 × 10^?13–1.06 × 10^?12	40