二维材料基超级电容器的容量与倍率性能提升策略

doi:10.1016/j.actphy.2025.100063

摘要/Abstract

摘要：

二维材料凭借其独特的层状结构、高比表面积、高理论容量和优异的柔韧性，成为构建高能量密度和高功率密度超级电容器电极的理想选择。然而，层间强范德华力导致的片层堆叠严重阻碍了离子传输，限制了其实际容量和倍率性能的发挥。因此，合理的材料设计和精细的电极结构调控对于突破超级电容器性能瓶颈至关重要。在这篇综述中，首先探讨了提升二维材料电化学性能的策略，重点阐述如何通过结构设计优化电极的面容量和体积容量。值得注意的是，提高超级电容器能量密度通常需要增加活性物质负载量，这不可避免地导致电极内部离子传输路径延长并复杂化，从而降低倍率性能。针对这一问题，我们回顾了传统的高负载电极离子传输通道构建方法，例如模板法、外场诱导组装和3D打印技术。然而，这些方法通常制备的孔道尺度在微米或亚微米级别，难以同时满足高倍率性能和高体积容量的要求。为同时实现高面容量、高体积容量和高倍率性能，本综述重点总结了近年来在构建纳米级孔道结构方面的创新方法，包括毛细管力致密化、层间嵌入、表面刻蚀和量子点策略等。这些方法致力于构建三维互联、高效的离子传输网络，从而推动高能量密度、高功率密度和小型化超级电容器技术的快速发展。

关键词: 超级电容器, 二维材料, 结构设计, 面容量, 体积容量, 倍率性能

Abstract:

With the profound transformation of the global energy landscape and the rapid advancement of portable electronic devices and electric vehicle industries, there is an increasingly urgent demand for high-performance energy storage devices. Among the available energy storage technologies, supercapacitors stand out due to their rapid charge/discharge capabilities, excellent cycling stability, and high power density, enabling reliable long-term operation as well as efficient energy conversion and storage. A fundamental challenge in contemporary energy storage research remains the enhancement of supercapacitor energy density while maintaining their inherent high power density capabilities. Two-dimensional (2D) materials have emerged as promising candidates for constructing high-performance supercapacitor electrodes. Materials such as graphene, transition metal nitrides and/or carbides (MXenes), and transition metal dichalcogenides possess unique layered structures with atomic thickness, exceptional surface areas, high theoretical capacities, and remarkable mechanical flexibility. These characteristics make them particularly suitable for developing next-generation energy storage devices. However, the inherent van der Waals interactions between nanosheets frequently result in restacking phenomena, significantly impeding ion transport and consequently limiting both practical capacity and rate performance. Thus, rational materials design and precise electrode architecture engineering are imperative for overcoming these performance limitations. This review first explores modification strategies for enhancing the electrochemical performance of 2D materials. Studies have shown that diverse modification approaches, including surface functionalization, defect engineering, and heterogeneous structure construction, can effectively increase active sites, enhance conductivity, and improve pseudocapacitive characteristics. These modifications lead to substantial improvements in both areal and volumetric capacitance of electrode materials. Notably, efforts to increase supercapacitor energy density typically necessitate higher active material mass loading, which inherently results in more complex and extended ion transport pathways within the electrode structure, thereby compromising rate performance. In addressing this challenge, we evaluate conventional methodologies for establishing ion transport channels in high mass loading electrodes, including template-based approaches, external field-induced assembly techniques, and three-dimensional (3D) printing processes. However, these traditional methods typically generate pore structures at the micrometer or sub-micrometer scale, making it challenging to simultaneously achieve optimal rate performance and volumetric capacitance. To concurrently optimize areal capacitance, volumetric capacitance, and rate performance, this review emphasizes recent innovative approaches for constructing nanoscale porous architectures. These include capillary force-driven densification, interlayer insertion strategies, surface etching techniques, and quantum dot methodologies. These advanced approaches aim to establish three-dimensional interconnected networks for efficient ion transport, thereby accelerating the development of miniaturized supercapacitor technologies that simultaneously achieve high energy density and high power density characteristics.

Key words: Supercapacitor, Two-dimensional material, Architecture design, Areal capacitance, Volumetric capacitance, Rate performance

刘华艳, 陈逸飞, 杨梦召, 顾佳俊. 二维材料基超级电容器的容量与倍率性能提升策略[J]. 物理化学学报, 2025, 41(6), 100063. doi: 10.1016/j.actphy.2025.100063

Huayan Liu, Yifei Chen, Mengzhao Yang, Jiajun Gu. Strategies for enhancing capacity and rate performance of two-dimensional material-based supercapacitors[J]. Acta Phys. -Chim. Sin. 2025, 41(6), 100063. doi: 10.1016/j.actphy.2025.100063

链接本文: https://www.whxb.pku.edu.cn/CN/10.1016/j.actphy.2025.100063

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I6/100063

图/表 11

表1

表2

Electrodes	Method	Electrolyte	Specific capacitance	Cycle stability	Ref.
V₂O₅/ Ti₃C₂T_x film	Self-assembly	1 mol∙L⁻¹ H₂SO₄	365 F∙g⁻¹ (10 mV∙s⁻¹) 211 F∙g⁻¹ (100 mV∙s⁻¹)	70.4%/5000	[99]
MnO₂/ Ti₃C₂T_x film	Self-assembly	1 mol∙L⁻¹ Na₂SO₄	315 F∙g⁻¹ (10 mV∙s⁻¹) 166 F∙g⁻¹ (100 mV∙s⁻¹)	98.3%/10000	[100]
MnO₂ film	Self-assembly	1 mol∙L⁻¹ Na₂SO₄	110 F∙g⁻¹ (10 mV∙s⁻¹) 32 F∙g⁻¹ (100 mV∙s⁻¹)	–	[100]
NGQDs modified NiCo-LDH/Ni(OH)₂ growth on carbon cloth	Self-assembly	6 mol∙L⁻¹ KOH	1833 F∙g^–1 (1 A∙g⁻¹)	–	[107]
NiCo-LDH/Ni(OH)₂ growth on carbon cloth	Self-assembly	6 mol∙L⁻¹ KOH	829 F∙g^–1 (1 A∙g⁻¹)	–	[107]
MnCo₂O₄/NG coated on nickel foam	Hydrothermal method	2 mol∙L⁻¹ KOH	1170 F∙g⁻¹ (1 A∙g⁻¹) 818 F∙g⁻¹ (20 A∙g⁻¹)	87.6%/10000	[102]
MnCo₂O₄ coated on nickel foam			940 F∙g⁻¹ (1 A∙g⁻¹) 323 F∙g⁻¹ (20 A∙g⁻¹)	53.1%/10000
NG coated on nickel foam			305 F∙g⁻¹ (1 A∙g⁻¹) 271 F∙g⁻¹ (20 A∙g⁻¹)	82.1%/10000
Cu₂O-CoO/GO pressed onto nickel foam	Hydrothermal method	6 mol∙L⁻¹ KOH	723 F∙g⁻¹ (1 A∙g⁻¹) 484 F∙g⁻¹ (10 A∙g⁻¹)	89.3%/10000	[101]
Cu₂O /GO pressed onto nickel foam			576 F∙g⁻¹ (1 A∙g⁻¹)	–
CoO/GO pressed onto nickel foam			533 F∙g⁻¹ (1 A∙g⁻¹)	–
MoS₂/WS₂/ rGO	Hydrothermal method	3 mol∙L⁻¹ KOH	365 F∙g⁻¹ (1 A∙g⁻¹) 281 F∙g⁻¹ (8 A∙g⁻¹)	66.0%/3000	[108]
MoS₂/rGO			161 F∙g⁻¹ (1 A∙g⁻¹)	–
WS₂/rGO			253 F∙g⁻¹ (1 A∙g⁻¹)	–
MnO₂/ Ti₃C₂T_x coated on nickel foam	Hydrothermal method	1 mol∙L⁻¹ Na₂SO₄	314 F∙g⁻¹ (1 A∙g⁻¹) 228 F∙g⁻¹ (8 A∙g⁻¹)	90.9%/5000	[104]
MnO₂ coated on nickel foam			148 F∙g⁻¹ (1 A∙g⁻¹) 73 F∙g⁻¹ (8 A∙g⁻¹)	69.9%/5000
Ti₃C₂T_x coated on nickel foam			137 F∙g⁻¹ (1 A∙g⁻¹) 64 F∙g⁻¹ (8 A∙g⁻¹)	59.5%/5000
NiCo-LDH/Ti₃C₂T_x	Hydrothermal method	6 mol∙L⁻¹ KOH	1030 F∙g⁻¹ (1 A∙g⁻¹) 628 F∙g⁻¹ (50 A∙g⁻¹)	80.1%/5000	[105]
NiCo-LDH	Hydrothermal method	6 mol∙L⁻¹ KOH	700 F∙g^–1 (1 A∙g⁻¹) 350 F∙g^–1 (50 A∙g⁻¹)	60.4%/5000	[105]
VO_x anchored Ti₃C₂T_x coated on graphite sheet	Hydrothermal method	0.5 mol∙L⁻¹ K₂SO₄	364 F∙g⁻¹ (1 A∙g⁻¹) 80 F∙g⁻¹ (15 A∙g⁻¹)	78.0%/10000	[109]
VO₂ coated on graphite sheet			245 F∙g⁻¹ (1 A∙g⁻¹)	–
Ti₃C₂T_x coated on graphite sheet			140 F∙g⁻¹ (1 A∙g⁻¹)	–
1T-MoS₂/Ti₃C₂ cast on carbon papers	Magneto-hydrothermal synthesis	1 mol∙L⁻¹ H₂SO₄	387 F∙g^–1 (1 A∙g⁻¹) 207 F∙g^–1 (50 A∙g⁻¹)	98.6%/10000	[110]
1T-MoS₂ cast on carbon papers			357 F∙g^–1 (1 A∙g⁻¹) 113 F∙g^–1 (50 A∙g⁻¹)	–
Ti₃C₂ cast on carbon papers			27 F∙g⁻¹ (1 A∙g⁻¹) 14.9 F∙g⁻¹ (50 A∙g⁻¹)	–
MoS₂/ MnO₂ coated on nickel foam	Hydrothermal method	0.5 mol∙L⁻¹ Na₂SO₄	277 F∙g⁻¹ (2 A∙g⁻¹) 136 F∙g⁻¹ (6 A∙g⁻¹)	89.0%/10000	[111]
MoS₂ coated on nickel foam			156 F∙g⁻¹ (2 A∙g⁻¹)	–
MnO₂ coated on nickel foam			215 F∙g⁻¹ (2 A∙g⁻¹)	–
MoS₂-MoO₂/G coated on nickel foam	Ball-milled + thermal treatment	1 mol∙L⁻¹ KOH	872 F∙g⁻¹ (1 A∙g⁻¹) 506 F∙g⁻¹ (10 A∙g⁻¹)	98.0%/3000	[103]
MoS₂ coated on nickel foam	Ball-milled + thermal treatment	1 mol∙L⁻¹ KOH	463 F∙g⁻¹ (1 A∙g⁻¹)	–	[103]

表2

图1

图2

图3

图4

表3

图5

图6

图7

图8

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2D materials	Electrical conductivity (S∙cm⁻¹)	Theoretical capacity (F∙g⁻¹)	Advantages	Disadvantages
Graphene [6–9]	~10⁶	550	Ultra-high conductivity; Excellent mechanical strength; Extremely high specific surface area; Excellent thermal conductivity; Good chemical stability.	Difficulty in functionalization and easy to reunion.
TMDs [10]	10^–4–10²	100–1700	Tunable bandgap; Excellent semiconductor properties; Abundant quantum states; Superior optoelectronic performance; Good catalytic activity.	Low electrical conductivity; Poor mechanical strength; Average chemical stability; Complex preparation; High cost.
TMOs [11–14]	10^–6–10^–2	1200–3500	Abundant redox reactions; Good catalytic performance; Lower cost.	Low electrical conductivity; Poor cycle stability; Weak mechanical properties; Low chemical stability.
MXene [15, 16]	10³–10⁴	300–500	High electrical conductivity; Excellent ion transport; Rich surface chemistry; Good hydrophilicity; Easy functionalization.	Poor air stability; Easily oxidizable; Difficult structural control.

Electrodes	Electrolyte	Mass loading (mg∙cm⁻²)	Density (g∙cm^–3)	Scan rate/Current density	gravimetric capacitance (F∙g^–1)	Areal capacitance (F∙cm^–2)	Volume capacitance (F∙cm^–3)	Ref.
V₂O₅/Ti₃C₂T_x	1 mol∙L⁻¹ H₂SO₄	10	1.25	10 A∙g⁻¹	147	1.47	184	[157]
GO	6 mol∙L⁻¹ KOH	86.76	1.58	15 A∙g⁻¹	164	14.29	259	[158]
Ti₃C₂T_x	3 mol∙L⁻¹ H₂SO₄	58.8	2.94	100 mV∙s⁻¹	78	4.59	230	[159]
Ti₃C₂T_x-GO	3 mol∙L⁻¹ H₂SO₄	1.16	3.31	2000 mV∙s⁻¹	222	0.26	736	[160]
Ti₃C₂T_x-GO	3 mol∙L⁻¹ H₂SO₄	1.00	3.1	1000 mV∙s⁻¹	205	0.21	634	[161]
Ti₃C₂T_x-NbN	1 mol∙L⁻¹ H₂SO₄	17.5	3.50	200 mV∙s⁻¹	79	1.38	276	[162]
Etched Ti₃C₂T_x	3 mol∙L⁻¹ H₂SO₄	9.1	3.1	1000 mV∙s⁻¹	64	0.57	197	[163]
Etched GO	EMIMBF₄/ACN	10.00	0.71	20 A∙g⁻¹	194	1.94	138	[127]
1T-MoS₂	0.5 mol∙L⁻¹ H₂SO₄	10.87	4.53	1000 mV∙s⁻¹	61	0.61	255	[164]
TALP	1 mol∙L⁻¹ Na₂SO₄	10.00	2.63	5 A∙g⁻¹	171	1.71	261	[165]

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