超级电容器用石墨烯薄膜：制备、基元结构及表面调控

doi:10.3866/PKU.WHXB202012085

Abstract

Abstract:

With the rapid development of the functional applications of portable and wearable electronic products (such as curved smartphones, smartwatches, laptops, and electronic skins), there is an urgent need to fabricate flexible, lightweight, and highly efficient energy storage devices that can provide sufficient power support. Flexible supercapacitors with high power density, high charging/discharging rates, wide operating temperature ranges, low maintenance consumption, and a long cycling lifespan can be integrated with smart wearable electronic products to provide power support. The conventional preparation method for the electrodes of flexible supercapacitors involves directly coating the active materials on flexible substrates. However, inactive materials such as the substrates and binders occupy a large volume and contribute notably to the weight of flexible electrodes, which is unsuitable for highly integrated flexible electronic devices. Owing to its unique characteristics, including large theoretical specific surface area, high electrical conductivity, excellent mechanical flexibility, good chemical stability, and ease of film processing, graphene has been widely used as an electrode material for flexible supercapacitors. The graphene film is a macrostructure with graphene nanosheets as the main structural units. As opposed to conventional flexible electrodes containing non-electrochemical active components such as collectors, conductive agents, and binders, graphene film electrodes are considered highly promising electrode materials for flexible supercapacitors because of their light weight and robust mechanical properties. However, the inevitable aggregation of graphene during electrode preparation creates ''dead volume'' in the film electrodes, where the electrolyte cannot reach, further limiting the specific capacitance. In this review, we review the recent research on graphene films used for flexible supercapacitors, with emphasis on the assembling methods for graphene films, regulation of the graphene units, and their electrochemical performance. First, simple preparation methods for graphene films are introduced: vacuum-assisted self-assembly, blade coating, pressing aerogel, wet spinning, and interfacial self-assembly. Second, two major strategies for structural control and surface modification of the graphene units are described in detail: (1) structural control can transform the two-dimensional graphene nanosheets into defect graphene, which not only weakens the van der Waals force and π–π bond interactions between the nanosheets, but also leads to the formation of three-dimensional conductive networks and ion transport channels during the assembly process; (2) surface modification, which can suppress the agglomeration of graphene nanosheets by introducing heteroatoms and reactive functional group molecules, while improving their electrical conductivity and wettability, and introducing pseudocapacitance. Finally, the persisting challenges and future development of the commercial applications of graphene films are discussed.

Key words: Graphene film, Supercapacitor, Preparation method, Structural regulation, Surface modification

Meihui Jiang, Lizhi Sheng, Chao Wang, Lili Jiang, Zhuangjun Fan. Graphene Film for Supercapacitors: Preparation, Foundational Unit Structure and Surface Regulation[J]. Acta Phys. -Chim. Sin. 2022, 38(2), 2012085. doi: 10.3866/PKU.WHXB202012085

Figures/Tables 11

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Table 1

Preparation, foundational unit structure regulation methods and electrochemical properties of graphene films."

Preparation	Regulation	Composition	Electrolyte	Electrochemical properties		Ref.
Preparation	Regulation	Composition	Electrolyte	Specific capacitance	Energy density	Ref.
Vacuum-assisted self-assembly	Pillared structure	EGM-rGO	EMIMBF₄	231 F·g^-1 at 1 A·g^-1	88.1 Wh·L^–1 at ~880 W·L^–1	82
	Pillared structure	GN/MCS	1 mol·L^-1 KOH*	211 F·g^-1 at 0.2 A·g^-1	–	22
	Pillared structure	GN/AC/MnO₂	PVA/Na₂SO₄	2.96 F·cm^–3 at 1 mA·cm^–2	0.27 mWh·cm^–3 at 2 mW·cm^–3	73
	Pillared structure	AC/CNT/RGO	1 mol·L^-1 LiClO₄ (EC/DEC = 1 : 1)	101 F·g^-1 at 0.2 A·g^-1	30 Wh·kg^-1 at ~2 kW·kg^-1	9
	Pillared structure	RGO/PPy/RGO	1 mol·L^-1 H₂SO₄	625.6 F·g^-1 at 0.22 A·g^-1	21.7 Wh·kg^-1 at 110 W·kg^-1	25
	Pillared structure & Porous structure	GNCN	1 mol·L^-1 Na₂SO₄	–	23.1 Wh·kg^-1 at 230.8 kW·kg^-1	91
	Pillared structure & Porous structure	PGF2-10	6 mol·L^-1 KOH*	318.8 F·cm^–3 at 1 A·g^-1		51
	Pillared structure & Porous structure	CNT/HGR	0.5 mol·L^-1 H₂SO₄*	268 F·g^-1 at 0.25 A·g^-1	–	23
	Porous structure	LGO20	PVA/H₃PO₄	149.7 mF·cm^–2 at 3 mV·s^–1	7.5 mWh·cm^–3 at 0.38 W·cm^–3	26
	Heteroatom doped	F-RGO-60	6 mol·L^-1 KOH	262.5 F·cm^–3 (178.6 F·g^–1) at 0.1 A·g^-1	9.14 Wh·L^–1 at 36.7 W·L^–1	24
Blade-coating	Ribbon-like structure	F-GRF	6 mol·L^-1 KOH	89.9 F·g^-1 at 2 mV·s^–1	12.5 Wh·kg^-1 at 89.9 W·kg^-1	60
	Heteroatom doped	I-rGO	PVA-KOH	450 mF·cm^–2 at 1 mA·cm^–2	~62 μWh·cm^-2 at 500 μW·cm^-2	16
	Pillared structure	PPDA-HGF	1 mol·L^-1 H₂SO₄ PVA-H₂SO₄	516 F·cm^–3 at 0.5 A·g^-1 19.6 F·cm^–3 at 1 A·g^-1	17.9 Wh·L^–1 at 430 W·L^–1 2.72 Wh·L^–1 at 146.5 W·L^–1	92
	Porous structure	Porous RGO	1 mol·L^-1 H₂SO₄	71 mF·cm^–2 at 1 mA·cm^–2	8.4 µWh·cm^-2 at 4900 μW·cm^-2	12
Pressing aerogel	Porous structure	HHG-PPy	1 mol·L^-1 Na₂SO₄	328 F·cm^–3 at 0.5 A·g^–1	22.3 Wh·L^–1 at 189.5 W·L^–1	30
Pressing aerogel	Porous structure	HGF	6 mol·L^-1 KOH EMIMBF₄/AN	310 F·g^-1 at 1 A·g^-1 298 F·g^-1 at 1 A·g^-1	–35 Wh·kg^-1 at ~260 W·L^–1	57
Wet spinning	Heteroatom doped & Functional modification	OAP/rGO	1 mol·L^-1 H₂SO₄	637 F·g^-1 at 1 A·g^-1	14.1 Wh·kg^-1 at 199.9 W·L^–1	17
	Crumpled structure & Heteroatom doped	NGF	1 mol·L^-1 H₂SO₄ EMIMBF₄	413 F·cm^–3 at 1 A·g^–1 380 F·cm^–3 at 1 A·g^–1	–161 Wh·L^–1 at 1435 W·L^–1	36
	Vertical orientation	GHF-HZ	1 mol·L^-1 H₂SO₄	211 F·g^-1 at 0.2 A·g^-1	–	37
Interfacial self-assembly	Porous structure	rHGF	1 mol·L^-1 H₂SO₄ PVA-H₂SO₄	244 F·cm^–3 at 0.1 A·g^–1 56 mF·cm^–2 at 0.1 mA·cm^–2	8.5 Wh·L^–1 at 14 W·L^–1 1.42 mWh·cm^-3 at 1.41 W·cm^-3	54
	Heteroatom doped	Cl-RGOF	KOH-PVA	2312 mF·cm^–2 at 1 mA·cm^–2	160.6 Wh·cm^–2 at 0.5 mW·cm^–2	102
	Crumpled structure	f-RGOF	1 mol·L^-1 H₂SO₄ PVA-H₂SO₄	238.4 F·g^-1 at 0.5 A·g^-1 208.8 F·g^-1 at 0.5 A·g^-1	8.3 Wh·kg^-1 at 250 W·kg^-1 1.7 mWh·cm^-3 at 60 mW·cm^-3	88
	Functional modification & Porous structure	DDDC-rGO	1 mol·L^-1 H₂SO₄ 1 mol·L^-1 TEA in AN	302 F·g^-1 at 1 A·g^-1 115 F·g^-1 at 2 A·g^-1	6.4 Wh·kg^-1 at 0.2 kW·kg^-1 29.3 Wh·kg^-1 at 1.1 kW·kg^-1	49
	Functional modification & Vertical orientation	DDDC-rGO	1 mol·L^-1 H₂SO₄	430 F·g^-1 at 0.5 A·g^-1	–	68
	Pillared structure	DA/rGO@PDA	1 mol·L^-1 H₂SO₄* 1 mol·L^-1 H₂SO₄	772.8 F·cm^–3 at 1 A·g^-1 4 F·cm^–3 at 0.5 A·g^-1	– 16.4 Wh·L^–1 at 218.8 W·L^–1	77

Table 1

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Graphene Film for Supercapacitors: Preparation, Foundational Unit Structure and Surface Regulation

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