同轴静电纺丝构筑微/纳米结构隔膜与电极材料用于锂离子电池：从原理到应用

doi:10.3866/PKU.WHXB202311030

物理化学学报 >> 2024, Vol. 40 >> Issue (10): 2311030.doi: 10.3866/PKU.WHXB202311030

同轴静电纺丝构筑微/纳米结构隔膜与电极材料用于锂离子电池：从原理到应用

李琪¹, 黎平安¹, 刘泽通¹, 张佳辉¹, 张浩¹, 余维来²^,*(), 胡先罗¹^,*()

¹ 华中科技大学材料科学与工程学院, 材料成形与模具技术全国重点实验室, 武汉 430074
² Department of Chemical Engineering, Stanford University, Stanford CA 94305, USA

收稿日期:2023-11-23 修回日期:2023-12-12 录用日期:2023-12-14 发布日期:2024-03-13
通讯作者: Email: huxl@mail.hust.edu.cn, Tel: +86-27-87558245 (胡先罗)wyyu@stanford.edu (余维来)
基金资助:
国家自然科学基金(52272206); 国家自然科学基金(51972132)

Fabricating Micro/Nanostructured Separators and Electrode Materials by Coaxial Electrospinning for Lithium-Ion Batteries: From Fundamentals to Applications

Qi Li¹, Pingan Li¹, Zetong Liu¹, Jiahui Zhang¹, Hao Zhang¹, Weilai Yu²^,*(), Xianluo Hu¹^,*()

¹ State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
² Department of Chemical Engineering, Stanford University, Stanford CA 94305, USA

Received:2023-11-23 Revised:2023-12-12 Accepted:2023-12-14 Published:2024-03-13
Contact: Email: huxl@mail.hust.edu.cn, Tel: +86-27-87558245 (Xianluo Hu)wyyu@stanford.edu (Weilai Yu)
Supported by:
the National Natural Foundation Science of China(52272206); the National Natural Foundation Science of China(51972132)

摘要/Abstract

摘要：

锂离子电池因其高能量密度、长循环寿命、优异的倍率性能和热稳定性而备受青睐，成为从便携式电子产品到电动汽车等实际应用中的最佳电源。在这种背景下，同轴静电纺丝技术因可制造适用于锂离子电池的独特纳米纤维材料而备受关注。尤其纤维材料具有高比表面积、高孔隙率、较大的长径比和易表面改性的优点，近年来在锂离子电池领域被广泛研究。这篇综述全面总结了同轴静电纺丝的基本原理与该技术在正极、负极和隔膜等锂离子电池关键材料中的实际应用和最新进展，并讨论了同轴静电纺纤维材料的纳米/微米结构决定其电化学性能的规律。此外，该综述还分析了同轴静电纺丝未来的发展方向，强调了未来拓展同轴静电纺丝技术在锂离子电池领域的应用所面临的挑战。

关键词: 锂离子电池, 同轴静电纺丝, 微/纳结构材料, 核-壳结构, 电化学性能

Abstract:

Highly coveted for their exceptional energy density, extended cycle life, impressive rate capability, and thermal stability, lithium-ion batteries (LIBs) stand out as the optimal power sources for real-world applications, ranging from portable electronics to electric vehicles (EVs). In this context, coaxial electrospinning has emerged as a compelling technique for fabricating nanofiber materials endowed with properties ideally suited for LIBs. These properties include a high specific surface area, exceptional porosity, a substantial aspect ratio, and facile surface modification. This comprehensive review encapsulates the fundamental principles, practical applications, and recent strides in coaxial electrospinning, particularly in the preparation of crucial LIB components such as cathodes, anodes, and separators. The intricate relationships between the micro/nanostructures of coaxially electrospun fiber materials and their resultant battery performances are meticulously examined. Additionally, the review outlines future directions and underscores the challenges inherent in advancing the field of coaxial electrospinning for LIBs.

Key words: Lithium-ion batteries, Coaxial electrospinning, Micro/nanostructured materials, Core-shell structures, Electrochemical performance

李琪, 黎平安, 刘泽通, 张佳辉, 张浩, 余维来, 胡先罗. 同轴静电纺丝构筑微/纳米结构隔膜与电极材料用于锂离子电池：从原理到应用[J]. 物理化学学报, 2024, 40(10), 2311030. doi: 10.3866/PKU.WHXB202311030

Qi Li, Pingan Li, Zetong Liu, Jiahui Zhang, Hao Zhang, Weilai Yu, Xianluo Hu. Fabricating Micro/Nanostructured Separators and Electrode Materials by Coaxial Electrospinning for Lithium-Ion Batteries: From Fundamentals to Applications[J]. Acta Phys. -Chim. Sin. 2024, 40(10), 2311030. doi: 10.3866/PKU.WHXB202311030

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202311030

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I10/2311030

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表1

Materials (core/shell)	Solvents (core/shell)	Fiber structures	Advantages	Electrochemical performance	Ref.
Core: mineral oil Shell: PAN	Mineral oil/N, N-dimethylformamide (DMF)	Core: covert to soft carbon Shell: covert to hard carbon	Core-shell carbon nanofibers	520 mAh∙g⁻¹ at 25 mA∙g⁻¹	72
Core: mineral oil Shell: PVP, nickel acetate Middle: PAN	Mineral oil/ DMF/DMF	Core: hollow Middle: amorphous carbon nanotubes Shell: hollow graphitic carbon nano-spheres after Ni removal	A novel architecture prepared by a novel triple-coaxial electrospinning technique	969 mAh∙g⁻¹ at 50 mA∙g⁻¹ volumetric capacity of ~1.4 Ah∙cm⁻³	81
Core: PAN Shell: PAN, PMMA	DMF/DMF	Core: carbon core Shell: porous carbon shell	Improving the mechanical properties of PCNFs with a dense amorphous carbon core	445.3 mAh∙g⁻¹ at 100 mA∙g⁻¹ after 100 cycles 388.9 mAh∙g⁻¹ at 1 A∙g⁻¹ after 1000 cycles	86
Core: Si NPs, PMMA Shell: PAN	Acetone, DMF/DMF	Core: Si NPs Shell: carbon shell	The carbon shell as a restriction boundary	1384 mAh∙g⁻¹ at 0.1C 721 mAh∙g⁻¹ at 12C	87
Core: SAN Shell: PAN	DMF/DMF	Core: hollow Shell: carbon shell	Investigating the effect of carbonization temperature on electrochemical performance	390, 334, 273, and 243 mAh∙g⁻¹ at 50 mA∙g⁻¹ (800, 1000, 1200, 1600 ℃)	78
Core: SAN Shell: SAN, PAN	DMF/DMF	Core: hollow Shell: porous carbon shell	Investigating the effect of pores on electrochemical performance	620 (pore) vs. 352 (no pore) mAh∙g⁻¹ at 50 mA∙g⁻¹ 77% after 10 cycles	79
Core: SAN, Si NPs Shell: PAN	DMF/DMF	Core: Si NPs Shell: carbon shell	In situ observation of contact-lithiation	596 mAh∙g⁻¹ at 50 mA∙g⁻¹ 92% after 50 cycles at 50 mA∙g⁻¹	73,88
Core: PMMA, Si NPs Shell: PVP	DMF/DMF	Core: Si NPs Shell: carbon shell	Excellent mechanical flexibility without compromising electrochemical performance	Initial reversible capacity of 1162.8 mAh∙g⁻¹ at 0.1 A∙g⁻¹ 762.0 mAh∙g⁻¹ after 100 cycles	90
Core: SAN, Si NPs, MWNT Shell: PAN	DMF/DMF	Core: Si NPs, MWNT Shell: carbon shell	MWNT as additional conductive paths between the Si NPs (excellent electrical conductivity)	911 mAh∙g⁻¹ at 50 mA∙g⁻¹	93
Core: PMMA, Si NPs, MXene Shell: PAN	DMF/DMF	Core: Si NPs, MXene Shell: carbon shell	MXene as a conductive substrate bridge the Si particles and carbon shell to form the conductive network	Initial reversible capacity of 1083 mAh∙g⁻¹ at 0.1 A∙g⁻¹ 301 mAh∙g⁻¹ at 2 A∙g⁻¹	95
Core: Si NPs, P(AN-co-MHI), PMMA Shell: P(AN-co-MHI), PMMA	DMF/DMF	Core: Si NPs, porous carbon Shell: porous carbon shell	Porous carbon in the core enables fast charge transfer, porous carbon shell shortens Li⁺ diffusion distance and facilitate ion transport	842.1 mAh∙g⁻¹ after 500 cycles at 0.5 A∙g⁻¹ 1366.6 mAh∙g⁻¹ at 0.5 A∙g⁻¹	96
Core: PAN-co-IA, thiourea, PMMA, porous Si NPs Shell: PAN-co-IA, thiourea, PMMA	DMF/DMF	Core: porous Si NPs Shell: sulfur-doped porous carbon shell	The porous structure of Si and carbon shell provides abundant diffusion channels for ion transport	excellent reversible capacity of 1112.7 mAh∙g⁻¹ after 1000 cycles at 2.0 A∙g⁻¹	97
Core: PAN Middle: SAN, Si NPs Shell: PAN	DMF/DMF/DMF	Core: carbon shell Middle: Si NPs Shell: carbon shell	The wire-in-tube-structured trilayered nanofibers	1211 mAh∙g⁻¹ at 50 mA∙g⁻¹ 75% after 100 cycles at 50 mA∙g⁻¹	94
Core: PMMA, zinc acetate Shell: PAN, graphene oxide (GO)	DMF/DMF	Core: ZnO NPs Shell: reduced GO incorporated glassy carbon	Enhancing battery performance by the incorporation of the reduced GO network into the shell	815 mAh∙g⁻¹ at 50 mA∙g⁻¹ 76% after 100 cycles	106
Core: PAN, PVP, Iron phytate NPs Shell: PAN, PVP, TiO₂	DMF/DMF	Core: Fe₂P NPs Shell: TiO₂/carbon shell	Carbon shell facilitates electron transport. TiO₂ shell inhibits the volume expansion and pulverization of the Fe₂P core.	Initial reversible capacity of 1175.7 mAh∙g⁻¹ 716.8 mAh∙g⁻¹ after 100 cycles	108
Core: PMMA, carboxyethyl germanium hemioxide Shell: PAN	DMF/DMF	Core: P/GeP NPs Shell: carbon shell	N-doped hollow carbon fibers that restrict the crystal growth and solve the volume expansion of P/GeP	Initial reversible capacity of 1340.9 mAh∙g⁻¹ 382.9 mAh∙g⁻¹ after 500 cycles at 1 A∙g⁻¹	109
Core: mineral oil Shell: phosphomolybdic acid, PAN	Mineral oil/DMF	Core: hollow Shell: Mo₂C@C NPs incorporated carbon shell	Manufacturing metal carbide/carbon composites by coaxial electrospinning	1176 mAh∙g⁻¹ at 100 mA∙g⁻¹ 674 mAh∙g⁻¹ after 300 cycles	107
Core: TEOS/PS Shell: PAN	HCl, DMF/ DMF	Core: SiO₂ shell Shell: N-doped carbon shell	Formation of hollow double-shelled PMo₁₂-SiO₂@N-C nanofibers	1641 mAh∙g⁻¹ after 1000 cycles at 2 A∙g⁻¹	111
Core: SAN, liquid metal nanoparticles (LMNPs), MWCNTs, GO Shell: PAN+SAN	DMF/DMF	Core: MWCNTs, rGO, self-healing LMNPs Shell: porous carbon shell	The LMNPs with a self-healing property and high theoretical capacity; MWCNTs and rGO as a conductive network	604 mAh∙g⁻¹ at 1000 mA∙g⁻¹ 552 mAh∙g⁻¹ after 1500 cycles 499 mAh∙g⁻¹ at 2000 mA∙g⁻¹	1
Core: SAN, Si NPs Shell: polyamic acid (PAA)	DMF/DMF	Core: Si NPs Shell: polyimide (PI)-based carbon shell	Investigating the relationship between electrochemical properties and different Si contents	621 mAh∙g⁻¹ at 100 mA∙g⁻¹ 77.8% after 200 cycles	92
Core: PAN, Mo(acac)₂ Shell: PMMA, TBT	DMF, acetic acid/DMF	MoO₃ encapsulated by TiO₂ layer incorporated porous carbon matrices	Enhancing the electrode conductivity by the CNFs matrices and the TiO₂ layers together	561 mAh∙g⁻¹ after 300 cycles at 1000 mA∙g⁻¹	103
Core: PEO Shell: PAN, PVP	DMF/DMF	N-enriched porous walnut anchored on carbon fibers	Synthesis of new structural N-rich carbon porous materials by coaxial electrospinning	965 mAh∙g⁻¹ at 200 mA∙g⁻¹ in the first cycle 99% after 30 cycles	84
Core: cellulose Shell: chitosan	EmimAc/ EmimAc	Bio-N-doped composite carbon nanofibrous mats	Investigating the effects of different electrospinning way	327 mAh∙g⁻¹ after 300 cycles at 100 mA∙g⁻¹ (single nozzle)	71
Core: PAN Shell: PVP, Ni(NO₃)₂	DMF/DMF	Core: carbon core Shell: Ni NPs	Improving the uniformity of catalyst and the controllability of catalyst content	546 mAh∙g⁻¹ after 100 cycles at 100 mA∙g⁻¹ 307 mAh∙g⁻¹ at 1 A∙g⁻¹	85
Core: PS Shell: copper acetate, PAN	DMF/DMF	Core: hollow Shell: conductive copper/carbon shell	Provides a cross-network for rapid electron diffusion and alleviates volume expansion	Initial capacity of 424 mAh∙g⁻¹ at 5 A∙g⁻¹ 378 mAh∙g⁻¹ after 1000 cycles	82
Core: PMMA, carboxyethyl germanium hemioxides Shell: PAN	DMF/DMF	Core: GeP NPs Shell: N-doped carbon shell	Overcoming difficulty in structural design and severe volume expansion of GeP	612 mAh∙g⁻¹ at the 600th cycle at 1 A∙g⁻¹	110

表1

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图13

表2

Materials (core/shell)	Solvents (core/shell)	Advantages	Thermal stability (shrinkage)	Ionic conductivity (mS·cm⁻¹)	Ref.
PDA, ODA/	Dimethylacetamide	PI: excellent thermal stability	0% at 150 ℃ for 1 h	1.68 (25 ℃)	137
PVDF-HFP	(DMAc)/DMF	PVDF-HFP: superior affinity with electrolyte		2.33 (40 ℃)
				3.44 (90 ℃)
Polyamic acid (PAA)/PVDF-HFP	DMAc/DMF	PI: outstanding thermal stability and self-extinguished properties PVDF-HFP: good affinity with liquid electrolyte	0% at 200 ℃ for 0.5 h	1.24	141
PSA/PVDF-HFP	DMAc/DMAc	PSA: excellent mechanical properties, thermal resistance PVDF-HFP: better anodic stability, good affinity with liquid electrolyte	0% at 200 ℃ for 0.5 h	1.97	125
Cellulose acetate/ PVDF-HFP	DMAc, acetone/DMAc, acetone	Cellulose core: high thermal stability PVDF-HFP shell: flame retardant	0% at 200 ℃ for 1 h	6.16	61
Cellulose acetate/PVDF-HFP, superfine LLTO NPs	DMAc, acetone/DMAc, acetone	LLTO NPs: retard the thermal degradation of cellulose		13.90 (20 ℃)	166
PLA/PBS	HFIP, CF, o-chlorobenzaldehyde/HFIP, CF, o-chlorobenzaldehyde	PLA: excellent thermo-dimensional stability, mechanical strength PBS: strong affinity, appropriate shut-down temperature	0% at 170 ℃ for 15 min	1.65	150
Mineral oil/ PVP, titanium tetraisopropanolate	-/Ethanol, acetic acid	Mineral oil: sacrifice material to form hollow fibers	Slight shrinkage at 500 ℃ for 3 h	1.41 (25 ℃)	159
PAN/PVDF-HFP	DMF/DMF	PAN: excellent flame-retardant property and high resistance to the effect of heat PVDF-HFP: an excellent polymer electrolyte material, inert; insoluble, and stable	0% at 150 ℃ for 30 min	1.74	143
PAN/PVDF-HFP	DMF/DMF	PAN: thermally stable, high mechanical strength PVDF-HFP: excellent electrolyte wettability	almost 0% at 250 ℃ for 10 min		142
PPESK/PVDF	N-methyl-2-pyrrolidone (NMP), tetrahydrofuran (THF)/DMAc, acetone	PPESK: novel soluble engineering plastics with a high glass transition temperature of 263–305 ℃ PVDF-HFP: as the thermal shutdown component	0% at 200 ℃ for 1 h	1.69	147
PMIA/PVDF	DMAc/DMAc, acetone	PMIA: high mechanical strength, excellent thermal stability PVDF: excellent anodic stability, polarity of electrolyte (high polarity C-F chemical bonds)	0% at 180 ℃ for 2 h	1.70	144
TPP/PVDF	DMF, acetone/acetone	TPP: flame retardant PVDF: encapsulation material, and melts at high temperature to release TPP		3.90	152
TPP/PVDF	DMF, acetone/acetone	TPP: flame retardant PVDF: encapsulation material, and melts at high temperature to release TPP, thermal shutdown		0.15–0.44	153
TPP/PVDF, SiO₂, GO	DMF, acetone/acetone	TPP: flame retardant PVDF: encapsulation material, and melts at high temperature to release TPP SiO₂ and GO: enhance thermal stability	3.79% at 150 ℃ for 1 h	0.88	154
PMIA/PVDF-HFP	DMAc, LiCl/DMF	PMIA: hard material, higher thermal stability, mechanical strength PVDF-HFP: soft material, higher electrochemical performance	0% at 180 ℃ for 1 h	0.68	146
PAN/PBS	DMF/HFIP, chloroform	PAN: good mechanical and thermal stability, fast Li⁺ transportation PBS: lower melting point than PE	0% at 200 ℃ for 15 min	2.10	151
PAN, HCNFs/ PVDF, UiO-66	DMAc, acetone/ DMAc, acetone	HCNFs: prevent membranes from serious shrinkage in the direction perpendicular UiO-66 NPs: increase the Li⁺ transport	0% at 200 ℃ for 1 h	1.59	169
PW/PAN	Kerosene/DMF	PW: remarkable latent heat (~240 J∙g⁻¹) and suitable phase transition temperature (~45 ℃) PAN: superior thermal stability and high electrolyte wettability	0% at 200 ℃	1.40	160
PW/PAN, BNNs	Kerosene/DMF	PW: absorb heat in situ PAN: superior thermal stability and high electrolyte wettability BNNs: promote heat conduction	0% at 200 ℃	0.84	161
PI/fluorinated PMIA	DMF/DMAc	PI: high wetting breaking strength suppress lithium dendrite F-PMIA: remarkable gelation degree	0% at 300 ℃	1.30	148
CNTs, PAN/ Uio-66-NH₂, PVDF-HFP	DMF/DMF, acetone	CNTs: hinder the displacement of PAN polymer chains and strengthen mechanical strength Uio-66-NH₂: improve the interfacial compatibility	15% at 150 ℃	3.43	171
PAN/PVDF	DMF/DMAc	PAN: excellent mechanical properties PVDF: promote the rapid migration of Li⁺, high electrode compatibility.	0% at 170 ℃ for 1 h	1.62	145
PMIA/PAN, PVDF-HFP, TiO₂	DMAc/DMF	PMIA and PAN: high thermal stability PVDF-HFP: high electrolyte affinity TiO₂: reinforce mechanical strength	0% at 220 ℃ for 1 h	1.36	149

表2

图14

表3

Materials (core/shell)	Solvents (core/shell)	Fiber structures	Advantages	Electrochemical performance	Ref.
Core: LiCoO₂ sol Shell: MgO sol	Distilled water	Core: partially oriented LiCoO₂ NPs Shell: poor crystallinity	Optimizing the influence of passivating surface film formed by MgO	The initial capacity of 192 mAh∙g⁻¹ 90% after 40 cycles	178
Core: LiNi_0.8Co_0.1Mn_0.1O₂ sol, PVP Shell: MgO sol	Distilled water	Core: LiNi_0.8Co_0.1Mn_0.1O₂ core Shell: MgO shell	A tubular structure composed of core-shell fibers with the addition of PVP	The initial capacity of 195 mAh∙g⁻¹ 89.2% after 50 cycles	31
Core: machine oil Shell: LiNiO₂ precursor	Distilled water	Core: hollow Shell: well-crystallized LiNiO₂	Preparing hollow nanofibers of continuous LiNiO₂ phase		177
Core: PVP Shell: LiFePO₄ precursor, AgNO₃, PVP	DMF/DMF	Core: hollow Shell: LiFePO₄/C/Ag	Contributes to the formation of conductive coating (PVP) and LiFePO₄ simultaneously	138.7 mAh∙g⁻¹ at 0.2C	179
Core: PMMA, LiFePO₄ precursor Shell: PAN	DMF/DMF	Core: hollow Shell: carbon fiber with integrated carbon-coated LiFePO₄ NPs.	High specific surface area hollow nanofibers with multiple active sites	153.2 mAh∙g⁻¹ at 0.2C 135.7 mAh∙g⁻¹ at 2C	180
Core: PMMA Shell: PAN	DMF/DMF	Core: hollow structure partially filled with S; Shell: microporous carbon fiber with integrated sulfur.	Alleviating the dissolution of soluble polysulfides, facilitating ion transport	Maximum capacity of 815 mAh∙g⁻¹ 88% after 70 cycles	190
Core: PMMA Shell: PAN	DMF/DMF	Core: hollow Shell: SnS₂	Restraining the shuttling effect of lithium polysulfides, facilitating the transport of ions and electrons	The initial capacity of 1138 mAh∙g⁻¹ at 0.2C, 675 mAh∙g⁻¹ after 500 cycles at 1C	185
Core: PMMA Shell: PAN	DMF/DMF	Core: hollow Shell: NiCo₂S₄	Restraining the shuttling effect of lithium polysulfides, facilitating ion/electron transport	The initial capacity of 1213 mAh∙g⁻¹ at 0.2C, 0.06% decay per cycle in 500 cycles at 1C	186
Core: PEO Shell: PAN	DMF/DMF	Core: hollow Shell: sulfurized PAN	Provides a 3D transmission path for ions and electrons; suppressing the shuttle effect	1250 mAh∙g_sulfur⁻¹ or 515 mAh∙g_electrode⁻¹ at 0.1C	187
Core: PMMA Shell: P(AN-co-MHI), PMMA, boric acid, TiO₂	DMF/DMF	Core: hollow Shell: TiO, boron-doped hollow multichannel carbon shell	Abundant void to alleviate the volume change of S and promote electrolyte infiltration, alleviating shuttle effect and improving electronic conductivity	1070 mAh∙g⁻¹ at 0.1 A∙g⁻¹, capacity decay rate of 0.096% per cycle over 300 cycles	188
Core: PMMA Shell: PAN, methyl methacrylate, PMMA, boric acid, SiO₂	DMF/DMF	Lotus-root-structure porous multichannel carbon nanotubes	Capturing sulfur and restricting its loss, facilitating the diffusion of lithium ions	778 mAh∙g⁻¹ after 100 cycles at 0.1C	189

表3

图15

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