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

物理化学学报 >> 2022, Vol. 38 >> Issue (2): 2012085.doi: 10.3866/PKU.WHXB202012085

所属专题：石墨烯的功能与应用

超级电容器用石墨烯薄膜：制备、基元结构及表面调控

姜美慧¹, 盛利志¹^,*(), 王超¹, 江丽丽², 范壮军³^,*()

¹ 北华大学木质材料科学与工程吉林省重点实验室，吉林吉林 132013
² 吉林化工学院材料科学与工程学院，吉林吉林 132022
³ 中国石油大学(华东)材料科学与工程学院，山东青岛 266580

收稿日期:2020-12-30 录用日期:2021-01-18 发布日期:2021-01-22
通讯作者: 盛利志,范壮军 E-mail:shengli_zhi@126.com;fanzhj666@163.com
作者简介:盛利志，1988年出生。2018年获哈尔滨工程大学博士学位; 现为北华大学副教授、硕士生导师。主要研究方向为纳米炭基材料可控制备及其在储能领域的应用
范壮军，2003年获中国科学院山西煤炭化学研究所博士学位; 现为中国石油大学(华东)教授、博士生导师。主要研究方向为纳米炭材料在储能、催化、环保领域的应用
基金资助:
国家自然科学基金(51902006);国家自然科学基金(51702117);国家自然科学基金(51672055);国家自然科学基金(51972342);泰山学者项目(ts20190922);山东省重大项目(ZR2019ZD51);吉林省科技发展计划(20190103034JH);吉林省科技发展计划(20180520014JH);吉林省青年人才托举工程(192009)

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

Meihui Jiang¹, Lizhi Sheng¹^,*(), Chao Wang¹, Lili Jiang², Zhuangjun Fan³^,*()

¹ Wood Material Science and Engineering Key Laboratory of Jilin Province, Beihua University, Jilin 132013, Jilin Province, China
² School of Materials Science and Engineering, Jilin Institute of Chemical Technology, Jilin 132022, Jilin Province, China
³ School of Materials Science and Engineering, China University of Petroleum, Qingdao 266580, Shandong Province, China

Received:2020-12-30 Accepted:2021-01-18 Published:2021-01-22
Contact: Lizhi Sheng,Zhuangjun Fan E-mail:shengli_zhi@126.com;fanzhj666@163.com
About author:Email: fanzhj666@163.com (Z.F.)
Email: shengli_zhi@126.com (L.S.)
Supported by:
the National Natural Science Foundation of China(51902006);the National Natural Science Foundation of China(51702117);the National Natural Science Foundation of China(51672055);the National Natural Science Foundation of China(51972342);the Taishan Scholar Project of Shandong Province(ts20190922);the Key Basic Research Projects of Natural Science Foundation of Shandong Province(ZR2019ZD51);Department of Science and Technology of Jilin Province(20190103034JH);Department of Science and Technology of Jilin Province(20180520014JH);the Young Elite Scientist Sponsorship Program by Jilin Province Science and Technology Association(192009)

摘要/Abstract

摘要：

石墨烯薄膜是一种以石墨烯纳米片为基元结构的宏观体，通过合理的结构设计和表面修饰使其具有优异的电学、力学和热学性能，将在电化学储能、电子器件、健康和环保等领域具有潜在的应用。本文主要综述了从石墨烯基元调控到二维宏观膜组装以及石墨烯薄膜在超级电容器应用中的研究进展。主要介绍了石墨烯薄膜的简易制备方法，并详细介绍了通过对石墨烯基元的结构调控和表面修饰来优化石墨烯薄膜电化学性能的两大策略，最后对石墨烯薄膜应用所面临的挑战和未来的发展进行了总结与展望。

关键词: 石墨烯薄膜, 超级电容器, 制备方法, 结构调控, 表面修饰

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

姜美慧, 盛利志, 王超, 江丽丽, 范壮军. 超级电容器用石墨烯薄膜：制备、基元结构及表面调控[J]. 物理化学学报, 2022, 38(2), 2012085. doi: 10.3866/PKU.WHXB202012085

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

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202012085

https://www.whxb.pku.edu.cn/CN/Y2022/V38/I2/2012085

图/表 11

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表1

石墨烯薄膜的制备、基元调控方法及电化学性能"

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

表1

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

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