锂离子电池氧化亚硅负极结构优化和界面改性研究进展

doi:10.3866/PKU.WHXB202103052

物理化学学报 >> 2022, Vol. 38 >> Issue (6): 2103052.doi: 10.3866/PKU.WHXB202103052

所属专题：面向电化学储能与转化的表界面工程

锂离子电池氧化亚硅负极结构优化和界面改性研究进展

朱思颖¹, 李辉阳¹, 胡忠利¹, 张桥保²^,*(), 赵金保¹, 张力¹^,*()

¹ 厦门大学化学化工学院，福建厦门 361005
² 厦门大学材料学院，福建厦门 361005

收稿日期:2021-03-24 录用日期:2021-04-25 发布日期:2021-04-29
通讯作者: 张桥保,张力 E-mail:zhangqiaobao@xmu.edu.cn;zhangli81@xmu.edu.cn
作者简介:张桥保，厦门大学材料学院副教授。2016获香港城市大学博士学位，2015年在佐治亚理工学院刘美林教授课题组访学，2016年至今在厦门大学工作。主要研究兴趣是二次电池关键电极材料的设计优化及其储能过程中的构效关系解析。
张力，厦门大学化学化工学院教授级高级工程师、博士生导师，嘉庚实验室研究员。重点围绕新材料规模化制备、电池界面优化以及储能新体系开展创新研究和应用开发。在Chem. Soc .Rev.、Adv. Mater.、Energy Environ.Sci.、Adv.Energy Mater.、ACS Nano、Adv. Funct. Mater.、Energy Storage Mater.等杂志以通讯作者发表论文近60篇。
基金资助:
国家自然科学基金(21875155);国家自然科学基金(52072323)

Research Progresses on Structural Optimization and Interfacial Modification of Silicon Monoxide Anode for Lithium-Ion Battery

Siying Zhu¹, Huiyang Li¹, Zhongli Hu¹, Qiaobao Zhang²^,*(), Jinbao Zhao¹, Li Zhang¹^,*()

¹ College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, China
² College of Materials, Xiamen University, Xiamen 361005, Fujian Province, China

Received:2021-03-24 Accepted:2021-04-25 Published:2021-04-29
Contact: Qiaobao Zhang,Li Zhang E-mail:zhangqiaobao@xmu.edu.cn;zhangli81@xmu.edu.cn
About author:Li Zhang, Email: zhangli81@xmu.edu.cn (L.Z.)
Qiaobao Zhang, Email: zhangqiaobao@xmu.edu.cn (Q.Z.)
Supported by:
the National Natural Science Foundation of China(21875155);the National Natural Science Foundation of China(52072323)

摘要/Abstract

摘要：

氧化亚硅(SiO)作为锂离子电池负极材料，具有较高的理论比容量(~2043 mAh·g^-1)以及合适的脱锂电位(< 0.5 V)，且原料储量丰富、制备成本较低、对环境友好，被认为是下一代高能量密度锂离子电池负极极具潜力的候选材料。然而，SiO在脱/嵌锂过程中存在着较严重的体积效应(~200%)，易导致材料颗粒粉化、脱落，严重影响了SiO负极电极的界面稳定性和电化学性能。近年来，人们围绕SiO负极结构优化和界面改性开展了大量工作。本文先从SiO负极材料的结构特点出发，阐述了该材料面临的主要瓶颈问题；继而从SiO的结构优化、SiO/碳复合和SiO/金属复合等三方面，系统总结了迄今已有的SiO负极结构设计和界面调控策略，并分别对其方法特点、电化学性能以及二者间关联规律进行了比较和归纳，最后对SiO负极材料结构和界面改性的未来发展方向进行了展望。

关键词: 锂离子电池, 氧化亚硅负极, 结构优化, 界面改性, 碳复合, 金属复合

Abstract:

Owing to the rapid development of scientific technology, the demand for energy storage equipment is increasing in modern society. Among the current energy storage devices, lithium-ion batteries (LIBs) have been widely used in portable electronics, handy electric tools, medical electronics, and other fields owing to their high energy density, high power density, long lifespan, low self-discharge rate, wide operating temperature range, and environmental friendliness. However, in recent years, with rapid development in various technological fields, such as mobile electronics and electric vehicles, the demand for batteries with much higher energy densities than the current ones has been increasing. Hence, the development of LIBs with a high energy density, prolonged cycle life, and high safety has become a focal interest in this field. To achieve the above objectives, it is important to strategically use novel anode materials with relatively high specific capacities. At present, artificial graphite is commonly used as an anode material for commercialized traditional LIBs, which can only deliver a practical capacity of 360–365 mAh·g^-1. Therefore, LIBs using graphite anodes have limited room for improvement in energy density. In the past two decades, considerable efforts have been devoted to silicon-based anode materials, which belong to the same family as carbon. To date, common silicon anode materials primarily include nano-silicon (nano-Si), silicon monoxide (SiO), suboxidized SiO (SiO_x), and amorphous silicon metal alloy (amorphous SiM). Among them, SiO has attracted the most attention for use as a negative electrode material for LIBs. As an anode for lithium-ion batteries (LIBs), silicon monoxide (SiO) has a high specific capacity (~2043 mAh·g^-1) and suitable charge (delithiation) potential (< 0.5 V). In addition, with the abundance of its raw material resource, low manufacturing cost, and environmental friendliness, SiO is considered a promising candidate for next-generation high-energy-density LIBs. Based on the testing of existing commercialized SiO materials, the reversible specific capacity of pure SiO can reach 1300–1700 mAh·g^-1. However, when acting as the anode for LIBs, SiO undergoes a severe volume change (~200%) during the lithiation/delithiation process, which can result in severe pulverization and detachment of the anode material. Meanwhile, lithium silicate and lithium oxide are irreversibly formed during the initial discharge–charge cycle. Moreover, the electrical conductivity of SiO is relatively low (6.7 × 10^-4 S·cm^-1). These shortcomings seriously impact the interfacial stability and electrochemical performance of SiO-based LIBs, leading to a low initial Coulombic efficiency and poor long-term cycling stability, which has significantly restricted its commercial application. In recent years, substantial efforts have been made on structural optimization and interfacial modification of SiO anodes. However, there is still a lack of a more comprehensive summary of these important developments. Therefore, this review aims to introduce the research work in this area for readers interested in this emerging field and to summarize in detail the research work on the performance optimization of SiO in recent years. Based on the structural characteristics of the SiO anode material, this review expounds the main challenges facing the material, and then summarizes the structural and interfacial modification strategies from the perspectives of SiO structure optimization, SiO/carbon composites, and SiO/metal composites. The methods and their features in all the studies are concisely introduced, the electrochemical performances are demonstrated, and their correlations are compared and discussed. Finally, we propose the development of the structural and interfacial optimization of the SiO anode in the future.

Key words: Lithium-ion battery, Silicon monoxide anode, Structure optimization, Interfacial modification, Carbon composites, Metal composites

朱思颖, 李辉阳, 胡忠利, 张桥保, 赵金保, 张力. 锂离子电池氧化亚硅负极结构优化和界面改性研究进展[J]. 物理化学学报, 2022, 38(6), 2103052. doi: 10.3866/PKU.WHXB202103052

Siying Zhu, Huiyang Li, Zhongli Hu, Qiaobao Zhang, Jinbao Zhao, Li Zhang. Research Progresses on Structural Optimization and Interfacial Modification of Silicon Monoxide Anode for Lithium-Ion Battery[J]. Acta Phys. -Chim. Sin. 2022, 38(6), 2103052. doi: 10.3866/PKU.WHXB202103052

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202103052

https://www.whxb.pku.edu.cn/CN/Y2022/V38/I6/2103052

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Sample	Initial discharge/charge specific capacity (mAh·g^-1)	ICE (%)	Cycling performance (mAh·g^-1)	Current density	Particle size	Year	Ref.
SiO/Graphite	951.1/770.4	81	762.0 (50 cycles)	0.1C	–	2007	38
SiO/C	1050/800	76	710 (100 cycles)	–	0.5–3 μm	2007	40
SiO/Graphite	1556/693	44.5	688 (30 cycles)	–	5–20 μm	2008	41
SiO/CNF	2027/724	35.7	675 (200 cycles)	0.1C	0.1–1 μm	2011	42
SiO	1779/1002	56.3	1000 (50 cycles)	100 mA·g^-1	< 10 μm	2013	39
F-doped SiO@C	1518/1050	70	975 (100 cycles)	400 mA·g^-1		2018	44

Sample	Initial discharge/charge specific capacity/(mAh·g^-1)	ICE (%）	Cycling performance (mAh·g^-1）	Current density	Particle size	Pore size	Year	Ref.
p-SiO	2250/1350	60	–	0.1C	–	–	2012	46
p-SiO@C	1990/1520	76.4	1490 (50 cycles)	0.1C	–	–	2013	47
p-SiO	2653/1709	64.4	1242 (100 cycles)	0.2C	< 20 μm	75.2 nm	2013	48
mp-SiO@N-doped C	1202/790	65.7	806 (250 cycles)	400 mA·g^-1	< 400 nm	v	2018	49
p-SiO@C	–	87	839.6 (110 cycles)	500 mA·g^-1	~60 μm	6.67 nm	2020	50
p-SiO@C	~1600/~1000	62	900 (200 cycles)	1000 mA·g^-1	–	2–15 nm	2020	51

Sample	Carbon precursor	Synthesis method	Initial discharge/charge specific capacity (mAh·g^-1)	ICE (%)	Cycling Performance (mAh·g^-1)	Current density	Particle size	Coating thickness	Conductive property	Year	Ref.
NC-SiO	EMI-DCA ion liquid	High-temperature carbonization	2024/1496	73.9	955 (100 cycles)	1C	–	20–30 nm	–	2013	70
SCG-5	Aniline, Graphite	In situ polymerization, Annealing	801/545	68	432 (500 cycles)	0.8C	1–10 μm	–	–	2017	64
SiO@C	Sodium dodecyl benzene sulfonate	Electrostatic force adsorption, Calcination	2205/1142	51.8	1085 (100 cycles)	0.1C	6 μm	7 nm	R = 329 Ω·sq^-1	2018	66
TC-SiO	Tetrabutyl titanate, Coal tar pitch	Calcination	1741/1252	71.9	674.5 (100 cycles)	0.14 A·g^-1	5–10 μm	4 nm	R_ct = 31.3 Ω	2018	65
SiO/NC	Melamine, Citric acid	Magnetic stirring, Sinter	1280/920	71	834 (150 cycles)	1000 mA·g^-1	–	15–20 nm	R_ct = 64.28 Ω	2019	68
SiO/NPC	Melamine, Phosphoric acid, Gelatin	Magnetic stirring, Sinter	1698/1223	72	847 (200 cycles)	1000 mA·g^-1	–	25–30 nm	R_ct = 33 Ω	2020	71
SiO/C	Glucose	Ball-milling, Calcination	1751/1259	71.9	850 (100 cycles)	200 mA·g^-1	–	–	–	2020	72
SiO/C/G	Asphalt, Graphite	Ball-milling, Spray drying, Pyrolysis	1509/963	63.8	950 (100 cycles)	100 mA·g^-1	15 μm	~10 nm	–	2020	73
SC-3	Bamboo charcoal	Ball-milling, Calcination, Aluminothermic reduction	2308/1260	56.3	1100 (300 cycles)	200 mA·g^-1	–	–	–	2020	74

Sample	Carbon precursor	Synthesis method	Initial discharge/ charge specific capacity (mAh·g^-1)	ICE(%)	Cycling performance (mAh·g^-1)	Current density	Particle size	Coating thickness	Conductive property	Year	Ref.
d-SiO@vG	CH₄	CVD	–	–	1600 (100 cycles)	–	–	–	R = 200 Ω·sq^-1	2017	75
SiO/CNT/C	C₂H₂, Asphalt	CVD	1259/1083	86	821.7 (200 cycles)	1 A·g^-1	10–20 μm	–	R_ct = 82.6 Ω	2019	76
SiO/C	CH₄	FTCVD	1463/1200	82	501 (300 cycles)	1.2 A·g^-1	6–7 μm	50 nm	R_ct = 53.39 Ω	2019	77
SiO/Graphite/C	Graphite, CH₄	FTCVD	930/800	86	799.1 (100 cycles)	200 mA·g^-1	12 μm	–	R_ct = 14.55 Ω	2019	78
SiO/1D-C/α-C	C₂H₂	FBCVD	1445/1012	70	893.6 (120 cycles)	0.1 A·g^-1	–	100 nm	R_ct = 170 Ω	2020	79
d-SiO/C @NCNB	C₂H₂, Hydroquinone, HCHO	CVD, Heat-treatment, Carbonization	1375/1004	73	1043 (100 cycles)	0.1C	5–18 μm	–	–	2020	80
SiO/G/CNT	Graphite, CH₄	Ball-milling, CVD	789/513	65	495 (100 cycles)	230 mA·g^-1	3 μm	–	R_ct = 44.16 Ω	2011	81
Si/SiO_x/C-3	Graphite	Ball-milling	882/649	73.6	726 (500 cycles)	0.1 A·g^-1	–	–	–	2017	82
SiO_x@NC	m-Phenylenediamine, Hexamethylenetetr amine, Pluronic F127	Ball-milling, Grinding, Annealing	1309/774	59.1	709 (100 cycles)	200 mA·g^-1	200–300 nm	40 nm	–	2020	83

	Carbon precursor	Synthesis methods	Advantages	Disadvantages
Wet chemical carbon coating	Organic solvents, ionic liquid	Stirring under heating, calcination	Abundant and cheap carbon sources; Simple and low-cost process; Various fabricating methods	The structure of carbon coat unlikely to be controlled due to the reactions in solvents; Consequent calcination after wet reaction increasing the whole cost; Toxic liquids produced from the reaction causing environmental pollution
Dry chemical carbon coating	C₂H₂, CH₄, asphalt, graphite	CVD, ball-milling	Technology being mature and available for large-scale manufacturing; easy to control the reaction and manipulate the carbon-coating structure; forthright process and mild conditions for solid reactions	High-cost and severe danger due to gas reactions; Toxic gases produced from the reaction causing expensive disposal and environmental pollution

锂离子电池氧化亚硅负极结构优化和界面改性研究进展

Research Progresses on Structural Optimization and Interfacial Modification of Silicon Monoxide Anode for Lithium-Ion Battery

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