导电金属有机骨架材料在超级电容器中的应用

doi:10.15541/jim20190433

无机材料学报 ›› 2020, Vol. 35 ›› Issue (7): 769-780.DOI: 10.15541/jim20190433 CSTR: 32189.14.10.15541/jim20190433

所属专题：能源材料论文精选(二)：超级电容器与储能电池(2020)；【虚拟专辑】超级电容器(2020~2021)

导电金属有机骨架材料在超级电容器中的应用

李泽晖¹,谭美娟²,郑元昊³,骆雨阳³,经求是³,蒋靖坤¹,李明杰⁴()

1. 清华大学环境学院, 环境模拟与污染控制国家重点联合实验室, 北京 100084
2. 南京信息工程大学环境科学与工程学院, 南京 210044
3. 清华大学材料学院, 北京 100084
4. 中国科学院青岛生物能源与过程研究所, 中科院生物基材料重点实验室, 青岛 266101

收稿日期:2019-08-16 修回日期:2019-09-29 出版日期:2020-07-20 网络出版日期:2019-10-23
作者简介:李泽晖(1991-), 男, 博士研究生. E-mail: lzh17@mails.tsinghua.edu.cn
LI Zehui(1991-), male, PhD candidate. E-mail: lzh17@mails.tsinghua.edu.cn
基金资助:
国家自然科学基金青年基金(51608509)

Application of Conductive Metal Organic Frameworks in Supercapacitors

LI Zehui¹,TAN Meijuan²,ZHENG Yuanhao³,LUO Yuyang³,JING Qiushi³,JIANG Jingkun¹,LI Mingjie⁴()

1. State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China
2. Nanjing University of Information Science and Technology, Nanjing 210044, China
3. School of Environmental Science and Engineering, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China
4. CAS Key Laboratory of Bio-based Materials, Qingdao Institute of Biomass Energy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China

Received:2019-08-16 Revised:2019-09-29 Published:2020-07-20 Online:2019-10-23
Supported by:
National Natural Science Foundation of China(51608509)

摘要/Abstract

摘要：

随着电子技术的持续发展, 对供电设备的要求也相应提高。超级电容器(SCs)具有较高的能量密度和优异的功率输出性能, 是新一代小型化、智能化、可穿戴电子设备的理想供电装置。开发能够快速充放电、性能稳定的SCs产品是储能领域的研究重点。电极材料作为SCs最重要的组成部分, 是进一步提升其性能的关键。导电金属有机骨架(MOFs)作为新型SCs电极材料, 具有规整的孔道结构、大比表面积、多种形貌及维度、可调控的导电性能等优异性质, 展现出巨大的潜力并引起了广泛关注。本文结合SCs的储能机理, 介绍了导电MOFs的结构、制备及导电机制, 进一步阐述了其作为SCs电极材料的设计策略, 重点综述了其在SCs领域的研究进展, 并展望了其应用前景与发展方向。

关键词: MOFs, 导电性, 超级电容器, 储能, 电极材料, 综述

Abstract:

With continuous development of electronics, the requirements for power supply systems are increasing. Supercapacitors (SCs), which have high energy density and excellent power output performance, are ideal power supplies for new generation of miniaturized, intelligent and wearable electronic devices. Thus, developing SCs with fast charge-discharge speed and high stability is a key research topic in the field of energy storage. As the most important part of SCs, electrode materials are critical to its performance. Due to the excellent performances of high-ordered pore structure, large specific surface area, diverse morphologies and dimensions, and adjustable conductivity, conductive metal-organic frameworks (MOFs) materials have shown great potential as promising SCs electrode materials, and have attracted wide attention. This review introduces the structure, conductive mechanism and preparation methods of conductive MOFs following a short introduction of SCs, describes its design strategy as SCs electrode materials, reviews the research progress of conductive MOFs in the field of SCs, and prospects its future application.

Key words: MOFs, conductivity, supercapacitor, energy storage, electrode material, review

中图分类号:

O614
O646

李泽晖,谭美娟,郑元昊,骆雨阳,经求是,蒋靖坤,李明杰. 导电金属有机骨架材料在超级电容器中的应用[J]. 无机材料学报, 2020, 35(7): 769-780.

LI Zehui,TAN Meijuan,ZHENG Yuanhao,LUO Yuyang,JING Qiushi,JIANG Jingkun,LI Mingjie. Application of Conductive Metal Organic Frameworks in Supercapacitors[J]. Journal of Inorganic Materials, 2020, 35(7): 769-780.

图/表 9

图1 MOF可能的电荷传输方式: (a)质子或电荷的跳跃, (b)空间穿越, (c)化学键或能带传输[22]

Fig. 1 Representation of possible modes of charge transport in MOFs: (a) hopping charge transport, (b) through-space charge transport, and (c) through-bond charge transport[22]

图2 导电MOFs电容器的调控策略

Fig. 2 Control strategy of conductive MOFs in supercapacitors From microstructure, active site, surface interface and nanocomposite of conductive MOFs to energy storage applications

图3 Cu-CAT NWAs的结构与性能比较图: (a)沿c轴观察的晶体结构; (b)固态超级电容器的结构(左)和由三个串联超级电容器供电的红色发光二极管的照片(右); (c, d)碳纤维纸上Cu-CAT NWAs纳米线的扫描电镜照片和实物照片(d内插图); (e)Cu-CAT NWAs和(f)MOF材料以及基于碳材料的对称固态超级电容器的性能比较[29]

Fig. 3 (a) Crystal structure of Cu-CAT viewed along the c-axis; (b) Structure of the solid-state supercapacitor (left) and photograph of a red light-emitting-diode powered by the three supercapacitors connected in series (right); (c, d) SEM and photographic images (inset in (d)) of the Cu-CAT NWAs growing on carbon fiber paper; Performance comparison of (e)Cu-CAT NWAs and (f) MOF materials, and carbon materials based symmetric solid-state supercapacitors[29]

图4 (a)二维MOFsNi3(HITP)2分子结构, (b)理想化Ni3(HITP)2的空间结构图, (c)其与不同材料的面积电容和比表面积比较[30]

Fig. 4 (a) Molecular structure of Ni3(HITP)2; (b) Relative size of pores, electrolyte Et4N+ and BF4- ions, and acetonitrile solvent molecules showing in a space-filling diagram of idealized Ni3(HITP)2; (c) Comparison of areal capacitance for various materials normalized relative to their BET surface areas[30]

表1 基于不同金属位点的MOFs及其电容性能

Table 1 MOFs with different center metal atoms for SCs

Metal	Organic ligand	MOFs	Conductivity /(S?m^-1)	S_BET/(m²·g^-1)	Specific capacitance	Energy density	Power density	Ref.
Fe	1,3,5-Benzenetricarboxylic acid (H₃BT)C	MIL-100	-	-	39 F·g^-1	-	-	[35]
Co	Polyethylene glycol (PEG)	Co-MOF-71	-	-	206.76 F·g^-1	7.18 Wh·kg^-1	-	[36]
Co	Benzendicarboxylic (BDC) acid	Co-BDC	-	9.09	131.8 F·g^-1	20.7 Wh·kg^-1	3880 W·kg^-1	[25]
Co	2,6-Naphthalenedicarboxylic (NDC) acid	Co-NDC	-	20.29	147.3 F·g^-1	23.1 Wh·kg^-1	5490 W·kg^-1	[25]
Co	4,4-Biphenyldicarboxylic (BPDC) acid	Co-BPDC	-	138.35	179.2 F·g^-1	31.4 Wh·kg^-1	5640 W·kg^-1	[25]
Ni	Isonicotinic acid	Ni-MOF	-	148	634 F·g^-1	-	-	[37]
Ni	Salicylate ion	1D Ni-MOF	-	186.8	1698 F·g^-1	-	-	[38]
Ni	p-Benzenedicarboxylic acid (PTA)	Ni-MOF-24	-	-	1127 F·g^-1	19.17 Wh·kg^-1	1750 W·kg^-1	[39]
Ni	1,3,5-Benzenetricarboxylic (btc) acid (H₃BT)C	Ni₃(btc)₂·12H₂O	-	-	726 F·g^-1	16.5 Wh·kg^-1	2078 W·kg^-1	[40]
Ni	9,10-Anthracenedicarboxylic acid (ADC)	Ni-DMOF-ADC	-	783	552 F·g^-1	-	-	[41]
Ni	2,3,6,7,10,11-Hexaiminotriphenylene (HITP)	Ni₃(HITP)₂	>5000	630	111 F·g^-1	-	-	[30]
Zn	4,4’-Biphenyldicarboxylic acid (H₂BPC)	Zn₆(BPC)₆(L)₃· 9DMF	-	-	23 F·g^-1	1.9 Wh·kg^-1	3 W·kg^-1	[42]
Zn	p-Phenylenediamine (pPDA)	Zn-(pPDA)MOF	0.1~1.05		200.86 F·g^-1	62.8 Wh·kg^-1	4500 W·kg^-1	[43]
Cd	2,5-Thiophenedicarboxylic acid (H₂TDC)	Cd₂(TDC)₂(L)₂· 2H₂O	-	-	22 F·g^-1	2.1 Wh·kg^-1	3.3 W·kg^-1	[42]
Zr	2,2’-Bipyridine-5,5’-dicarboxylate (BPYDC)	nMOF-867	-	-	5.085 mF·cm^-2	6.04× 10^-4 Wh?cm^-3_stack	1.097 W·cm^-3_stack	[44]
Zn, Ni	p-Benzenedicarboxylic acid (PTA)	Zn-doped Ni-MOF	-	-	1620 F·g^-1	27.56 Wh·kg^-1	1750 W·kg^-1	[45]
Co, Zn	Benzendicarboxylic acid	Co8-MOF-5	-	2900	0.49 F·g^-1	-	-	[46]
Zn, Zr	Terephthalic acid	HP-UiO-66	-	-	849 F·g^-1	32 Wh·kg^-1	240 W·kg^-1	[47]

表1 基于不同金属位点的MOFs及其电容性能

Table 1 MOFs with different center metal atoms for SCs

Metal	Organic ligand	MOFs	Conductivity /(S?m^-1)	S_BET/(m²·g^-1)	Specific capacitance	Energy density	Power density	Ref.
Fe	1,3,5-Benzenetricarboxylic acid (H₃BT)C	MIL-100	-	-	39 F·g^-1	-	-	[35]
Co	Polyethylene glycol (PEG)	Co-MOF-71	-	-	206.76 F·g^-1	7.18 Wh·kg^-1	-	[36]
Co	Benzendicarboxylic (BDC) acid	Co-BDC	-	9.09	131.8 F·g^-1	20.7 Wh·kg^-1	3880 W·kg^-1	[25]
Co	2,6-Naphthalenedicarboxylic (NDC) acid	Co-NDC	-	20.29	147.3 F·g^-1	23.1 Wh·kg^-1	5490 W·kg^-1	[25]
Co	4,4-Biphenyldicarboxylic (BPDC) acid	Co-BPDC	-	138.35	179.2 F·g^-1	31.4 Wh·kg^-1	5640 W·kg^-1	[25]
Ni	Isonicotinic acid	Ni-MOF	-	148	634 F·g^-1	-	-	[37]
Ni	Salicylate ion	1D Ni-MOF	-	186.8	1698 F·g^-1	-	-	[38]
Ni	p-Benzenedicarboxylic acid (PTA)	Ni-MOF-24	-	-	1127 F·g^-1	19.17 Wh·kg^-1	1750 W·kg^-1	[39]
Ni	1,3,5-Benzenetricarboxylic (btc) acid (H₃BT)C	Ni₃(btc)₂·12H₂O	-	-	726 F·g^-1	16.5 Wh·kg^-1	2078 W·kg^-1	[40]
Ni	9,10-Anthracenedicarboxylic acid (ADC)	Ni-DMOF-ADC	-	783	552 F·g^-1	-	-	[41]
Ni	2,3,6,7,10,11-Hexaiminotriphenylene (HITP)	Ni₃(HITP)₂	>5000	630	111 F·g^-1	-	-	[30]
Zn	4,4’-Biphenyldicarboxylic acid (H₂BPC)	Zn₆(BPC)₆(L)₃· 9DMF	-	-	23 F·g^-1	1.9 Wh·kg^-1	3 W·kg^-1	[42]
Zn	p-Phenylenediamine (pPDA)	Zn-(pPDA)MOF	0.1~1.05		200.86 F·g^-1	62.8 Wh·kg^-1	4500 W·kg^-1	[43]
Cd	2,5-Thiophenedicarboxylic acid (H₂TDC)	Cd₂(TDC)₂(L)₂· 2H₂O	-	-	22 F·g^-1	2.1 Wh·kg^-1	3.3 W·kg^-1	[42]
Zr	2,2’-Bipyridine-5,5’-dicarboxylate (BPYDC)	nMOF-867	-	-	5.085 mF·cm^-2	6.04× 10^-4 Wh?cm^-3_stack	1.097 W·cm^-3_stack	[44]
Zn, Ni	p-Benzenedicarboxylic acid (PTA)	Zn-doped Ni-MOF	-	-	1620 F·g^-1	27.56 Wh·kg^-1	1750 W·kg^-1	[45]
Co, Zn	Benzendicarboxylic acid	Co8-MOF-5	-	2900	0.49 F·g^-1	-	-	[46]
Zn, Zr	Terephthalic acid	HP-UiO-66	-	-	849 F·g^-1	32 Wh·kg^-1	240 W·kg^-1	[47]

图5 nMOF-867的结构及nMOFs作为电极的SCs的性能[44]

Fig. 5 Structure of MOF‐867 and performance of the nMOF SCs[44]

图6 所有基于Ni-DMOFs在电流密度为10 A?g-1时, 非对称SCs的循环性能[41]

Fig. 6 Cycle performance for all Ni-DMOFs-based asymmetric supercapacitor at a current density of 10 A?g-1[41]

图7 纽扣电池型超级电容器的结构示意图[44]

Fig. 7 Schematic diagram for coin-type supercapacitors[44]

图8 (a)碳布上聚苯胺-ZIF-67的合成示意图, (b)PANI-ZIF-67-CC与其他电极材料的面积电容对比, (c~f)组装成全固态SCs示意图及(g)由串联的三个SCs供电的红色发光二极管(LED)的照片[52]

Fig. 8 (a) Illustration of the synthesis methodology for polyaniline-ZIF-67 on carbon cloth; (b) Areal capacitances of the PANI-ZIF-67-CC and other electrode materials; (c-f) Schematic illustrations of PANI-ZIF-67-CC flexible solid-state SC device; (g) Photograph of a red light-emitting-diode (LED) powered by the three SCs connected in series[52]

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导电金属有机骨架材料在超级电容器中的应用

Application of Conductive Metal Organic Frameworks in Supercapacitors

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