炭-/石墨烯量子点在超级电容器中的应用

doi:10.3866/PKU.WHXB201903052

物理化学学报 >> 2020, Vol. 36 >> Issue (2): 1903052.doi: 10.3866/PKU.WHXB201903052

所属专题：超级电容器

炭-/石墨烯量子点在超级电容器中的应用

朱家瑶¹,董玥²,张苏^1,*(),范壮军^3,*()

¹ 新疆大学，能源材料化学教育部重点实验室，先进功能材料自治区重点实验室，应用化学研究所，乌鲁木齐 830046
² 北京化工大学，化工资源有效利用国家重点实验室，材料电化学过程与技术北京重点实验室，北京 100029
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:2019-03-25 录用日期:2019-04-25 发布日期:2019-05-08
通讯作者: 张苏,范壮军 E-mail:suzhangs@163.com;fanzhj666@163.com
作者简介:张苏，男，1989年生。分别于2011年、2016年在北京化工大学获得学士和博士学位，师从宋怀河教授。现为新疆大学应用化学研究所副教授，主要从事炭材料及其在超级电容器、锂离子电池方面的应用研究|范壮军，男，中国石油大学(华东)教授，2003年博士毕业于中国科学院山西煤炭化学研究所，曾获国家“万人计划”科技创新领军人才，省部级科技一等奖两项。目前主要从事纳米炭材料在储能、催化、环保领域的应用基础研究
基金资助:
国家自然科学基金(51702275);国家自然科学基金(51672055);新疆高校科研计划(XJEDU2017S003)

Application of Carbon-/Graphene Quantum Dots for Supercapacitors

Jiayao Zhu¹,Yue Dong²,Su Zhang^1,*(),Zhuangjun Fan^3,*()

¹ Key Laboratory of Energy Materials Chemistry, Ministry of Education, Key Laboratory of Advanced Functional Materials, Autonomous Region, Institute of Applied Chemistry, Xinjiang University, Urumqi 830046, P. R. China
² State Key Laboratory of Chemical Resource Engineering, Beijing Key Laboratory of Electrochemical Process and Technology for Materials, Beijing University of Chemical Technology, Beijing 100029, P. R. China
³ School of Materials Science and Engineering, China University of Petroleum, Qingdao 266580, Shandong Province, P. R. China

Received:2019-03-25 Accepted:2019-04-25 Published:2019-05-08
Contact: Su Zhang,Zhuangjun Fan E-mail:suzhangs@163.com;fanzhj666@163.com
Supported by:
the National Natural Science Foundation of China(51702275);the National Natural Science Foundation of China(51672055);the Scientific Research Program of the Higher Education Institution of Xinjiang, China(XJEDU2017S003)

摘要/Abstract

摘要：

炭-/石墨烯量子点作为新兴的炭纳米材料，因具有独特的小尺寸效应和丰富的边缘活性位点而在高性能超级电容器电极材料的研发方面展现出巨大潜力。针对目前炭-/石墨烯量子点在超级电容器电极材料方面的应用优势和存在的关键问题，本文以炭-/石墨烯量子点、量子点/导电炭复合材料、量子点/金属氧化物复合材料、量子点/导电聚合物复合材料以及量子点衍生炭这些电极材料为脉络，梳理了近年来该领域的发展状况，尝试阐释炭-/石墨烯量子点在电极材料、复合材料和衍生炭电极材料中所起到的关键作用，最后对炭-/石墨烯量子点电极材料的发展进行了展望。本综述以期为炭-/石墨烯量子点基电极材料的研究提供一定参考和依据。

关键词: 炭量子点, 石墨烯量子点, 超级电容器, 复合材料, 炭材料

Abstract:

Supercapacitors have attracted considerable attention as new-generation energy storage devices because of their high charge-discharge rate, ultralong lifetime, and high power density. However, the performance of supercapacitors is severely restricted by either the low intrinsic capacitance of porous carbons or the poor conductivity and sluggish electrochemical kinetics of pseudocapacitive components. Therefore, high-performance electrode materials integrated with high gravimetric and volumetric capacitances, high rate capability, and superb cycling stability are urgently needed. As emerging carbon nanomaterials, carbon-/graphene quantum dots (CDs/GQDs) have uniquely small particle sizes, abundant edge sites, and various functional groups, thus endowing them with great potential for developing high-performance electrode materials for supercapacitors. With the purpose of identifying the application advantages and critical problems of CDs/GQDs for supercapacitor electrodes, this review summarizes the development of CDs/GQDs, quantum dots (QDs)/conductive carbon, QDs/metal oxides, QDs/conductive polymer composites, and QD-derived carbon materials in recent years. In each section of this paper, we introduce the typical and updated studies from corresponding fields in terms of novel preparation routes, the crucial roles of CDs/GQDs in composite materials, and the electrochemical performance of electrode materials and assembled devices. Finally, the advantages and limitations of CD/GQD electrode materials are described, and the future development of QD-based materials is discussed. In general, the previous studies have shown that when directly used as electrode materials for micro-supercapacitors, CDs/GQDs performed at an ultrahigh charge-discharge rate of up to 1000 V∙s⁻¹. However, because of the discontinuous conductive network and good dispersibility in electrolytes, they are not suitable for use in common devices because of poor cycle stability. One of the most promising means for fully realizing active ion storage sites for portable devices is to strongly anchor CDs/GQDs onto conductive carbon scaffolds such as activated carbon, graphene nanosheets, and carbon nanofibers. QDs simultaneously improve the capacitive and rate performance owing to the active sites and improved surface wettability of the composite materials. To further improve the capacitance and cycle stability of electrode materials, different types of QDs/pseudocapacitive material composites (metal oxides or conductive polymers) have been developed. QDs have been shown to increase entire conductivity, accelerate ion transport, and depress the volume expansion of metal oxides and conductive polymers. Benefiting from their small-sized structure and outstanding reactivity, CDs/GQDs can also be used as emerging precursors for constructing advanced carbon electrode materials. Several forward-looking studies have shown that QDs can be converted to carbon nanosheets, heteroatom-doped carbon, and dense and porous carbon blocks with high gravimetric/volumetric capacitances and remarkable rate performance for fast and compact energy storage. Although related fields have rapidly developed in recent years, several critical problems including those related to green and effective methods to prepare CDs/GQDs, construction of entire conductive networks without active sites being sacrificed, the synergistic effect, and the underlying mechanism of QDs in composite materials still must be solved. We hope that this review can provide inspiration and references for further investigation in this promising field.

Key words: Carbon quantum dot, Graphene quantum dot, Supercapacitor, Composite, Carbon material

朱家瑶, 董玥, 张苏, 范壮军. 炭-/石墨烯量子点在超级电容器中的应用[J]. 物理化学学报, 2020, 36(2), 1903052. doi: 10.3866/PKU.WHXB201903052

Jiayao Zhu, Yue Dong, Su Zhang, Zhuangjun Fan. Application of Carbon-/Graphene Quantum Dots for Supercapacitors[J]. Acta Physico-Chimica Sinica 2020, 36(2), 1903052. doi: 10.3866/PKU.WHXB201903052

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB201903052

https://www.whxb.pku.edu.cn/CN/Y2020/V36/I2/1903052

图/表 10

图1

图2

表1

炭-/石墨烯量子点-导电炭复合电极材料超级电容器的性能"

Materials	Methods	Interaction	Function of CD/GQD	Specific surface area (m².g⁻¹)	Specific capacitance	Rate capability	Electrolyte	Testing system	Ref.
CD/graphene oxide	microfluid spinning	hydrogen bond	pillar	435.1	91.9 F∙g⁻¹@ 0.1 mA∙cm⁻²	60.1 F∙g⁻¹@ 1 mA∙cm⁻²	H₂SO₄/PVA	solid	48
CD/activated carbon	sonication	–	–	723	134 F∙g⁻¹@ 1 A∙g⁻¹	95 F∙g⁻¹@ 50 mV∙s⁻¹	6 mol∙L⁻¹ KOH	two electrode	51
GQD/carbonized MOF-5	electrochemical deposition	–	providing pseudocapacitance, increasing surface wettability	704.2	780 F∙g⁻¹@ 10 mV∙s⁻¹	–	1 mol∙L⁻¹ H₂SO₄	three electrode	54
GQD/carbonized MOF-5	electrochemical deposition	–	providing pseudocapacitance, increasing surface wettability	704.2	294.1 F∙g⁻¹@ 0.5 A∙g⁻¹	195.8 F∙g⁻¹@ 20 A∙g⁻¹	1 mol∙L⁻¹ H₂SO₄	two electrode	54
GQD/graphene hydrogel	electrochemical deposition	–	providing sub-nanometer pores	292	268 F∙g⁻¹@ 1.25 A∙g⁻¹	130 F∙g⁻¹@ 5 A∙g⁻¹	1 mol∙L⁻¹ H₂SO₄	two electrode	55
GQD/porous graphene oxide	ozone treatment	chemical bond	pillar	7.24	353 F∙g⁻¹@ 2 mV∙s⁻¹	234 F∙g⁻¹@ 500 mV∙s⁻¹	6 mol∙L⁻¹ KOH	three electrode	49
GQD/porous graphene oxide	ozone treatment	chemical bond	pillar	7.24	69.7 F∙g⁻¹@ 2 mV∙s⁻¹	26.2 F∙g⁻¹@ 500 mV∙s⁻¹	1 mol∙L⁻¹ Na₂SO₄	two electrode	49
GQD/graphene	electrochemical deposition	metal chelating/coordination	–	–	7.02 μF∙cm⁻²@ 0.02 μA∙cm⁻²	3.22 μF∙cm⁻²@ 0.03 μA∙cm⁻²	H₂SO₄/PVA	solid	47
GQD/carbon nanofiber	low temperature synthesis	covalent ester bond	providing active sites	–	213 F∙g⁻¹@ 1 A∙g⁻¹	31 F∙g⁻¹@ 10 A∙g⁻¹	1 mol∙L⁻¹ H₂SO₄	two electrode	52
GQD/chitosan-derived carbon	carbonization	–	–	–	545 F∙g⁻¹@ 1 A∙g⁻¹	175 F∙g⁻¹@ 20 A∙g⁻¹	1 mol∙L⁻¹ H₂SO₄	three electrode	58
CD/polyacrylamide-derived carbon	carbonization	–	–	1025	468 F∙g⁻¹@ 1 A∙g⁻¹	374 F∙g⁻¹@ 30 A∙g⁻¹	3 mol∙L⁻¹ KOH	three electrode	59
					510 F∙g⁻¹@ 1 A∙g⁻¹	398 F∙g⁻¹@ 30 A∙g⁻¹	4 mol∙L⁻¹ H₂SO₄	three electrode
					438 F∙g⁻¹@ 1 A∙g⁻¹	312 F∙g⁻¹@ 30 A∙g⁻¹	1 mol∙L⁻¹ Li₂SO₄	three electrode
N-doping GQD/carbonized MOF-8-CNT	electrochemical deposition	–	providing pseudocapacitance, increasing wettability	520	540 F∙g⁻¹@ 0.5 A∙g⁻¹	332.1 F∙g⁻¹@ 20 A∙g⁻¹	1 mol∙L⁻¹ H₂SO₄	two electrode	56
CD/reduced graphene oxide	hydrothermal deposition	–	pillar	44.52	308 F∙g⁻¹@ 0.5 A∙g⁻¹	222 F∙g⁻¹@ 20 A∙g⁻¹	6 mol∙L⁻¹ KOH	three electrode	57
GQD/carbon nanotube/carbon cloth	electrochemical deposition	–	increasing interface interaction	–	592.8 mF∙cm⁻²@ 0.5 mA∙cm⁻²	461 mF∙cm⁻²@ 20 mA∙cm⁻²	H₂SO₄/PVA	solid	53
N-doping GQD/ graphene oxide	optical reduction	–	pillar	–	344 F∙g⁻¹@ 0.25 A∙g⁻¹	210 F∙g⁻¹@ 4.17 A∙g⁻¹	6 mol∙L⁻¹ KOH	three electrode	50
GQD/glucosamine hydrochloride	hydrothermal-carbonization	–	improving conductivity	2829	388 F∙g⁻¹@ 1 A∙g⁻¹	233 F∙g⁻¹@ 100 A∙g⁻¹	6 mol∙L⁻¹ KOH	two electrode	60

表1

图3

图4

表2

炭-/石墨烯量子点-赝电容组分复合电极材料"

Materials	Methods	Influence on morphologies	Electrolyte	Specific capacitance	Cycle stability	Function of CD/GQD	Ref.
CD/RuO₂	mixing	–	1 mol∙L⁻¹ H₂SO₄	594 F∙g⁻¹@1 A∙g⁻¹ 460 F g⁻¹@50 A∙g⁻¹	97% @ 5000 cycles @ 5 A∙g⁻¹	improving conductivity		69
CD/Ni(OH)₂	hydrothermal treatment	control morphology change	2 mol∙L⁻¹ KOH	2750 F∙g⁻¹@1 A g⁻¹, 1763 F∙g⁻¹@20 A∙g⁻¹	96% @ 2000 cycles @ 20 A∙g⁻¹	improving conductivity, inducing morphology change, accelerating ion transport		63
CD/NiCo₂O₄	reflux-heat treatment	–	2 mol∙L⁻¹ KOH	856 F∙g⁻¹@1 A∙g⁻¹ 520 F∙g⁻¹@100 A∙g⁻¹	99% @ 10000 cycles @ 5 A∙g⁻¹	improving conductivity		72
CD/NiCo₂O₄	hydrothermal-air heat treatment	control morphology change	3 mol∙L⁻¹ KOH	2168 F∙g⁻¹@1 A∙g⁻¹, 1620 F∙g⁻¹@30 A∙g⁻¹	No fading @ 5000 cycles @ 30 A∙g⁻¹	inducing morphology change, accelerating ion transport, increasing wettability		73
CD/MnO₂	hydrothermal treatment	control morphology change	1 mol∙L⁻¹ Na₂SO₄	340 F∙g⁻¹@1 A∙g⁻¹ 260 F∙g⁻¹@20 A∙g⁻¹	76% @ 10000 cycles @ 1 A∙g⁻¹	improving conductivity and wettability		70
GQD/MnO₂	plasma enhanced chemical vapor deposition	Mn-O-C bond	1 mol∙L⁻¹ Na₂SO₄	1094 F∙g⁻¹@5 mV∙s⁻¹, 380 F∙g⁻¹@100 mV∙s⁻¹	95% @ 10000 cycles @ 1 A∙g⁻¹	improving conductivity and stability		71
GQD/halloysite nanotubes	electrostatic assembly	–	1 mol∙L⁻¹ Na₂SO₄	323 F∙g⁻¹@5 mV∙s⁻¹, 186 F∙g⁻¹@100 mV∙s⁻¹, 363 F∙g⁻¹@0.5 A∙g⁻¹, 216 F∙g⁻¹@20 A∙g⁻¹	88% @ 5000 cycles @ 6 A∙g⁻¹	accelerating ion transport		62
N-doped GQD /Fe₃O₄/halloysite nanotubes	electrostatic assembly	–	1 mol∙L⁻¹ Na₂SO₄	370 F∙g⁻¹@5 mV ∙s⁻¹, 210 F∙g⁻¹@100 mV∙s⁻¹, 418 F∙g⁻¹@0.5 A∙g⁻¹, 130 F∙g⁻¹@10 A∙g⁻¹	83% @ 3000 cycles @ 1 A∙g⁻¹	accelerating ion transport		61
GQD/polyaniline	mixed oxidation-polymerization	control morphology change	0.5 mol∙L⁻¹ H₂SO₄	1044 F∙g⁻¹@1 A∙g⁻¹, 635 F∙g⁻¹@10 A∙g⁻¹	80% @ 3000 cycles @ 1 A∙g⁻¹	increase structural stability, accelerating ion transport		74
CD/polyaniline	mixed oxidation-polymerization	control morphology change	1 mol∙L⁻¹ H₂SO₄	970 F∙g⁻¹@1 A∙g⁻¹, 610 F∙g⁻¹@20 A∙g⁻¹	85% @ 2000 cycles @ 10 A∙g⁻¹	improving structural stability and conductivity		75
CD/polyaniline	electrochemical polymerization	–	1 mol∙L⁻¹ H₂SO₄	738 F∙g⁻¹@1 A∙g⁻¹, 495 F∙g⁻¹@10 A∙g⁻¹	78% @ 1000 cycles @ 5 A∙g⁻¹	increase structural stability, accelerating ion transport		76
CD/polypyrrole	electrostatic adsorption	–	1 mol∙L⁻¹ KCl	306 F∙g⁻¹@0.5 A∙g⁻¹, 210 F∙g^-1 @ 40 A∙g^-1	85% @ 5000 cycles @ 5mA∙cm⁻²	Increase structural stability, accelerating ion transport		77
graphene aerogel /CD/CuS	hydrothermal-heat treatment	–	6 mol∙L⁻¹ KOH	782 F∙g⁻¹@1 A∙g⁻¹, 410 F∙g⁻¹@10 A∙g⁻¹	80% @ 5000 cycles @ 5 A∙g⁻¹	increasing interface bonding, providing pseudocapacitance		79
Graphene/CD/ MnO_x	low temperature chemical reduction	reductant, crystalline core	1 mol∙L⁻¹ Na₂SO₄	480 F∙g⁻¹@0.2 A∙g⁻¹, 100 F∙g⁻¹@1.25 A∙g⁻¹	94.7% @ 10000 cycles @ 1.2 A∙g⁻¹	protecting graphene structure		80
graphene aerogel/CD/MnO₂	hydrothermal-oxidation	reducing MnO₂ particle sizes	1 mol∙L⁻¹ Na₂SO₄	721 F∙g⁻¹@1 A∙g^W#8722;1, 643 F∙g⁻¹@20 A∙g⁻¹	92% @ 10000 cycles @ 10 A∙g⁻¹	increasing interface bonding and stability		81
graphene oxide/CD/polypyrrole	blending polymerization	–	1 mol∙L⁻¹ LiCl	576 F∙g⁻¹@0.5 A∙g⁻¹, 488 F∙g⁻¹@10 A∙g⁻¹	93% @ 1000 cycles @ 10 A∙g⁻¹	increasing interface bonding and dielectrical property		78

表2

图5

图6

图7

图8

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Application of Carbon-/Graphene Quantum Dots for Supercapacitors

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