可拉伸超级电容器的研究进展:电极、电解质和器件

邵光伟; 郭珊珊; 于瑞; 陈南梁; 叶美丹; 刘向阳

doi:10.7498/aps.69.20200881

摘要

可拉伸超级电容器因在可穿戴电子和健康监测等领域的潜在应用而受到人们的广泛关注, 它不但具备普通超级电容器功率密度高、循环寿命长、安全、成本低等优点, 而且良好的柔软性和可拉伸性使其能够很好地与可穿戴系统进行集成. 本文对已有文献中可拉伸电极/器件的制备方法进行归类、分析, 详细总结了可拉伸电极/器件的三种制备方法, 即弹性聚合物基底、可拉伸结构设计以及弹性聚合物和可拉伸结构结合; 另外, 还介绍了多功能可拉伸超级电容器和高弹性凝胶电解质的研究进展; 最后, 分析总结了可拉伸超级电容器未来发展中仍需面临的一些挑战. 期望能够激发更多的研究创造以推动可拉伸超级电容器的实际应用.

关键词:

超级电容器 /
可拉伸 /
电极 /
电解质

Abstract

Stretchable supercapacitors have received more and more attention due to their potential applications in wearable electronics and health monitoring. The stretchable supercapacitors have not only the advantages of high power density, long cycle life, safety and low cost of ordinary supercapacitor, but also good flexibility and stretchability to integrate well with wearable system. In this review, according to the structures of supercapacitors, the methods of preparing stretchable electrodes/devices reported in the literature are categorized and analyzed. We particularly highlight the key findings of creating stretchable electrodes/devices, which include elastic polymer substrates, tensile structure design and elastic polymer + tensile structure. In addition, the research progress of multi-functional stretchable supercapacitors and high elastic gel electrolytes are discussed. Finally, the challenges to the future development of the stretchable supercapacitors are analyzed and summarized. We expect to stimulate more research in creating stretchable supercapacitors for wide practical applications.

Keywords:

作者及机构信息

1.
东华大学纺织学院, 上海市高性能纤维复合材料省部共建协同创新中心, 产业用纺织品教育部工程研究中心, 上海　201620

2.
厦门大学物理科学与技术学院, 生物仿生及软物质研究院, 厦门　361005

3.
新加坡国立大学理学院, 新加坡　119077

通信作者: 于瑞, yurui@xmu.edu.cn ; 陈南梁, nlch@dhu.edu.cn ; 叶美丹, mdye@xmu.edu.cn ; 刘向阳, phyliuxy@nus.edu.sg

基金项目: 国家级-中央高校基本科研业务费专项资金、东华大学研究生创新基金资助(CUSF-DH-D-2019046)

Authors and contacts

1.
Shanghai Collaborative Innovation Center for High Performance fiber composites, Engineering Research Center of Technical Textile, Ministry of Education, College of Textiles, Donghua University, Shanghai 201620, China

2.
Research Institute for Biomimetics and Soft Matter, College of Physical Science andTechnology, Xiamen University, Xiamen 361005, China

3.
Faculty of Science, National University of Singapore, Singapore 119077, Singapore

Corresponding author: Yu Rui, yurui@xmu.edu.cn ; Chen Nan-Liang, nlch@dhu.edu.cn ; Ye Mei-Dan, mdye@xmu.edu.cn ; Liu Xiang-Yang, phyliuxy@nus.edu.sg

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施引文献

图 1 充放电原理示意图　(a) 双电层电容器; (b) 赝电容电容器; (c) 混合型电容器. (d) 超级电容器的结构示意图

Fig. 1. Schematic illustrations of energy storage mechanisms of (a) electric double-layer capacitor, (b) pseudocapacitor, (c) hybrid capacitor. (d) Structure diagram of supercapacitor.

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图 2 可拉伸超级电容器的设计思路: 弹性聚合物、可拉伸结构以及两者的结合

Fig. 2. Design ideas of stretchable supercapacitor: Elastic polymer, stretchable structure, and elastic polymer + stretchable structure.

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图 3 弹性聚合物为基底材料制备的可拉伸电极/器件　(a), (b) PDMS基底^[36,50]; (c) Ecoflex基底^[52]; (d) PU基底^[21]; (e) 弹性纤维基底^[55]

Fig. 3. Stretchable electrodes/supercapacitors based on elastic polymer: (a), (b) PDMS^[36,50]; (c) Ecoflex^[52]; (d) PU^[21]; (e) elastic fiber^[55].

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图 4 可拉伸结构设计制得的电极/器件　(a) 螺旋结构^[66]; (b) 波浪结构^[68]; (c) 织物结构^[71]; (d) 蛇形结构^[75]; (e)−(g) 网状结构^[45,76,78]

Fig. 4. Stretchable supercapacitors based on stretchable structure: (a) Helical structure^[66]; (b) wave structure^[68]; (c) fabric structure^[71]; (d) serpentine structure^[75]; (e)−(g) net structure^[45,76,78].

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图 5 织物结构可拉伸超级电容器　(a)织物结构可拉伸超级电容器示意图; (b)可拉伸织物结构示意图; (c)不可拉伸织物结构示意图; (d)可拉伸织物结构实物图; (e)不同应变(10%, 20%和30%)和8 A/g电流密度情况下, 不同拉伸/释放循环次数后的电容量保持率(插图为拉伸循环期间可拉伸超级电容器的实物图); (f)在肘部放置可拉伸超级电容器的示意图; 两个放置于肘部并串联的可拉伸超级电容器用于点亮肘部的LED灯泡的实物图: (g)胳膊拉伸和(h)胳膊弯曲; (i)两个串联的器件可以点亮40个组装成“DHU”字母的LED灯泡^[81]

Fig. 5. Schematic illustrations of stretchable supercapacitors: (a) Fabric structure stretchable supercapacitors; (b) stretchable fabric structure; (c) non-stretchable fabric structure; (d) image of stretchable fabric structure; (e) capacity retention after different numbers of stretch/release cycles under different strains (10%, 20%, and 30%) at a current density of 8 A/g (the inset presents the images of the hybrid supercapacitor device during stretching cycles); (f) schematic of elbow-fitted supercapacitor; images of two supercapacitors connected in series for the illumination of an elbow-fitted LED for (g) stretching and (h) bending. (i) Two devices connected in series for the illumination of a set of 40 LEDs with a parallel "DHU" pattern^[81].

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图 6 织物结构可拉伸超级电容器与文献中报道的超级电容器在拉伸恢复率、拉伸循环稳定性和电化学性能等方面的比较, 其中C0和C分别对应于拉伸循环前后的比容量

Fig. 6. Comparison of the stretchable supercapacitor with reported supercapacitors with respect to the tensile recovery, stretching cyclic stability, and electrochemical properties, where C0 and C correspond to the specific capacities before and after stretching cycles, respectively.

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图 7 弹性聚合物和可拉伸结构组合制备的可拉伸复合电极/器件　(a), (b) 弹性聚合物和波浪结构^[57,92]; (c) 弹性聚合物和螺旋结构^[94]; (d) 弹性聚合物和织物结构^[97]; (e) 弹性聚合物和网状结构^[59]

Fig. 7. Stretchable supercapacitors based on elastic polymer and stretchable structure: (a), (b) Elastic polymer and wave structure^[57,92]; (c) elastic polymer and helical structure^[94]; (d) elastic polymer and fabric structure^[97]; (e) elastic polymer and net structure^[59].

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图 8 可拉伸超级电容器的多功能性　(a) 自供电^[47]; (b) 传感^[73]; (c), (d)透明^[87,120]

Fig. 8. Multifunction stretchable supercapacitors: (a) Self-powered^[47]; (b) sensing^[73]; (c), (d) transparent^[87,120].

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图 9 可拉伸超级电容器的多功能性　(a)−(e) 超薄^[112]; (f) 自愈合^[90]

Fig. 9. Multifunction stretchable supercapacitors: (a)−(e) ultrathin^[112]; (f) self-healing^[90].

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图 10 高弹性凝胶电解质　(a), (b) 琼脂/HPAAm双网络水凝胶^[126]; (c) H₃PO₄-聚乙烯醇(PVA)聚合物凝胶电解质^[105]

Fig. 10. (a) Illustration of the preparation of Agar/HPAAm double-net hydrogel; (b) the recovery performance of Agar/HPAAm hydrogel and Agar/PAAm hydrogel under different stretching conditions^[126]; (c) schematic configuration of the intrinsically stretcha-ble supercapacitor using highly stretchable gel electrolyte^[105].

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表 1 利用弹性聚合物为基底制备可拉伸超级电容器的研究概括

Table 1. Summary of recent studies on stretchable supercapacitor based on elastic polymer.

导电处理	活性材料	沉积方法	电容表现	极限拉伸率/%	电容稳定性	文献
PDMS基底材料的可拉伸超级电容器
石墨烯	石墨烯	激光诱发	650 μF/cm² @35 μA/cm²	50	1000次拉伸循环后保持84%电容	[35]
碳纳米管	V₂O₅/PEDOT	旋涂	135 mF/cm² @0.5 mA/cm²	50	100次拉伸循环后保持85%电容	[36]
单壁碳纳米管	单壁碳纳米管	化学汽相淀积	17.5 F/g	120	1000次拉伸循环后电容没有变化	[50]
单壁碳纳米管	单壁碳纳米管/ 氮化硼纳米管	干压	7.7 F/g @19 μF/cm²	50	50%应变下1000次拉伸循环后电容增加25%	[51]
PU基底材料的可拉伸超级电容器
聚吡咯	聚吡咯	化学聚合	108.5 F/g@1 A/g	100	100%应变下拉伸1000次后保持90%电容	[37]
氮-碳纳米管	氮-碳纳米管	化学气相沉积	37.6 mF/cm² @0.05 mA/cm²	500	1000次拉伸后保持96%电容	[21]
Ecoflex基底材料的可拉伸超级电容器
碳纳米管	单壁碳纳米管	涂覆	15.2 F/cm³ @0.021 A/cm³	60	在0, 20%, 40%应变下, 1000次充放电循环后电容保持97.4%, 95.5%, 94.5%	[52]
PEDOT:PSS基底材料的可拉伸超级电容器
银掺杂	PEDOT:PSS/碳纳米管	浸渍烘干	64 mF/cm² (85.3 F/g)	480	400%应变下100次拉伸循环后保持90%电容	[53]
多壁碳纳米管	多米碳纳米管@聚苯胺	电聚合	2.2 F/cm³ @1 mA/cm²	50	50%应变下300次拉伸循环后CV曲线没有明显变化	[54]

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表 2 通过可拉伸结构设计制备可拉伸超级电容器的研究概括

Table 2. Summary of recent studies on stretchable supercapacitors based on stretchable structure.

导电处理	活性材料	沉积方法	电容表现	极限拉伸率/%	电容稳定性	文献
螺旋结构设计的可拉伸超级电容器
不锈钢弹簧	碳纳米管/聚苯胺	原位合成	277.8 F/g@1 A/g, 402.8 mF/cm @1 mA/cm	100	在100%应变下电容没有明显降低	[41]
碳纳米管纱线	聚吡咯/碳纳米管	电沉积	63.6 F/g@1 A/g	150	—	[42]
不锈钢线	MnO₂/还原氧化石墨烯	电沉积	2.86 mWh/cm³	400	400%应变下拉伸循环3000次后保持95%电容	[64]
碳纳米管纱线	碳纳米管纱线/MnO₂/聚吡咯	电沉积	60.43 mF/cm², 7.72 F/g, 9.46 F/cm³, 9.86 mF/cm@10 mV/s	20	20%应变下拉伸循环200次后保持88%电容	[65]
碳纳米管纤维	碳纳米管	纺丝	0.51 mF/cm, 27.07 mF/cm² @150 mA/cm³	300	拉伸循环300次后保持94%电容	[66]
波浪结构设计的可拉伸超级电容器
碳纳米管	碳纳米管@MnO₂/碳纳米管@聚吡咯	电沉积	2.2 F/cm³ @2 mA/cm²	100	拉伸循环500次后保持96%电容	[67]
泡沫镍	聚苯胺/石墨烯	电聚合	261 F/g	30	30%应变下拉伸循环100次后保持95%电容	[68]
织物结构设计的可拉伸超级电容器
银涂层	聚吡咯@MnO₂	丝网印刷	0.0337 mWh/cm², 95.3 mF/cm²@5 mV/s	40	40%应变下保持 86.2%电容	[69]
不锈钢网	聚吡咯	电化学沉积	170 F/g@0.5 A/g	20	20%应变下拉伸循环10000次后保持87%电容	[46]
碳纳米管织物	聚吡咯@MnO₂	电镀	461 F/g@0.2 A/g	21	21%应变下保持98.5%电容	[70]
碳纤维	PEDOT:PSS/碳	浸渍涂覆	—	100	100%应变下拉伸循环6000次后保持70%电容	[71]
导电过滤网	聚吡咯@MnO₂	电沉积	—	20	—	[29]
银镀层	MnO₂–碳纳米管/PEDOT:PSS	丝网印刷	17.5 mWh/cm² @0.4 mW/cm²	20	20%应变下拉伸循环100次后保持95.26%电容	[47]
单壁碳纳米管	单壁碳纳米管	浸渍烘干	140 F/g, 0.48 F/cm²@20 μA/cm²	120	拉伸后比电容没有变化	[72]
多壁碳纳米管	多壁碳纳米管/MoO₃	喷涂	48.3 F/g@0.14 A/g, 33.8 mF/cm² @0.1 mA/cm	50	应变从10%增加到50%, 拉伸循环5000次后保持80%电容	[73]
蛇形结构设计的可拉伸超级电容器
钛/铂	聚吡咯-多壁碳纳米管	喷涂	5.17 mF/cm² @100 μA/cm²	30	30%应变下双轴拉伸循环1000次后充放电行为没有发生明显变化	[74]
单壁碳纳米管	单壁碳纳米管	喷涂	100 μF@0.5 V/s	30	30%应变下拉伸循环10次后电容没有明显恶化	[75]
网状结构设计的可拉伸超级电容器
单壁碳纳米管膜	单壁碳纳米管	喷涂	1.6 F/cm³, 448 nF/cm² @1 V/s	150	150%应变下电容保持不变	[44]
碳纳米管膜	聚吡咯/黑磷/碳纳米管	电沉积	7.35 F/cm² @7.8 mA/cm²	2000	2000%应变下拉伸循环10000次后保持95%电容	[76]
碳纳米管	碳纳米管/聚吡咯	电沉积	69 F/g, 3.5 mF/cm, 74.1 mF/cm², 9.9 F/cm³ @2 mV/s	10	5%应变下拉伸循环5000次后有101%动态电容	[77]
碳纳米管膜	碳纳米管	化学气相沉积	61.4 mF/cm², 35.7 F/g 16.0 F/cm³@1 mA/cm²	16	16%应变下拉伸循环3000次后保持93.3%电容	[45]
碳纳米管	MnO₂/碳纳米管	水热合成法	227.2 mF/cm²	500	400%应变下拉伸循环10000次后保持98%电容	[78]

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表 3 弹性聚合物与可拉伸结构结合的复合电极制备可拉伸超级电容器研究概括

Table 3. Summary of recent studies on stretchable supercapacitors based on elastic polymer + stretchable structure.

基底材料	结构类型	导电处理	活性材料	沉积方法	电容表现	拉伸率/%	电容稳定性	文献
PDMS	波浪结构	多壁碳纳米管	多壁碳纳米管/聚苯胺	3D打印	44.13 mF/cm²@ 0.2 mA/cm²	40	在5%-40%不同应变情况下, 电化学性能几乎没有变化	[57]
PDMS	波浪结构	3D-石墨烯	3D-石墨烯/聚苯胺	原位聚合	77.8 Wh/kg @995 W/kg	100	100%应变下拉伸循环100次后保持91.2%电容	[60]
PDMS	波浪结构	碳纳米管	聚苯胺/碳纳米管	涂覆	308.4 F/g@8 A/g	100	100%应变下拉伸循环200次后电容保持不变	[82]
PDMS	波浪结构	单壁碳纳米管/PEDOT 混合纤维	单壁碳纳米管/PEDOT	电沉积	53 F/g, 1.6 mF/cm²@1 A/g	100	X和Y两个方向, 100%应变下拉伸循环5000次后保持96.9% 和 90.1%电容	[83]
PDMS	波浪结构	碳纳米管膜	MnO₂/碳纳米管, Fe₂O₃/碳纳米管	水热反应	45.8 Wh/kg	100	在多种应变下电化学循环10000次后保持98.9%电容	[62]
PDMS	波浪结构	不锈钢线	Ni-Co-S/还原氧化石墨烯	电沉积	127.2 mF/cm² @0.1 mA/cm	100	100%应变下拉伸循环1000次后保持91%电容	[84]
PDMS	波浪结构	单壁碳纳米管/聚苯胺混合膜	单壁碳纳米管/聚苯胺	化学气相沉积	106 F/g@1 A/g	120	拉伸循环200次后保持85%电容	[85]
PDMS	网状结构	还原氧化石墨烯	还原氧化石墨烯	浸渍烘干	188 mAh/g @0.05 A/g	50	50%应变下拉伸循环100次后保持89%电容	[86]
PDMS	网状结构	金-聚甲基丙烯酸甲酯PMMA 纳米纤维网	MnO₂	电沉积	3.68 mF/cm² @0.007 mA/cm²	60	60%应变下保持92%电容	[59]
PDMS	网状结构	银/金核壳纳米线	聚吡咯	电化学沉积	580 μF/cm² @5.8 μA/cm²	50	应变从10%增加到50%, CV曲线几乎没有变化	[87]
PDMS	网状结构	泡沫石墨烯	聚吡咯/ 石墨烯	化学气相沉积和化学界面聚合	258 mF/cm² @1 mA/cm²	50	30%应变下充放电循环100次后保持88%电容	[80]
PU	螺旋结构	镀银	碳纳米管	浸渍涂覆	4.17 mWh/cm³	150	重复拉伸变形后电容没有明显下降	[58]
PU	螺旋结构	碳纳米管	聚吡咯/碳纳米管	电沉积	69 mF/cm²	130	应变从0%增加到40%, 拉伸循环1000次后保持85%电容	[88]
PU	螺旋结构	纳米碳	N-石墨烯/3D镍钴铝	原位聚合	1.1 mWh/cm² @2.59 mW/cm²	100	50%应变下拉伸循环10000次后保持91%电容	[89]
PU	螺旋结构	还原氧化石墨烯纤维	聚吡咯/还原氧化石墨烯/多壁碳纳米管		0.94 mWh/cm³	100	100%应变下保持82.4%电容	[90]
Ecoflex 橡胶芯	螺旋结构	碳纳米管	MnO₂/PEDOT@碳纳米管	电沉积	2.38 mF/cm, 11.88 mF/cm²	200	在拉伸循环和扭曲循环后电容分别保持92.8%和98.2%	[91]
Ecoflex	波浪结构	泡沫镍	聚苯胺/ 石墨烯	电沉积	261 F/g@0.38 A/g	30	30%应变下拉伸循环100次后保持95%电容	[68]
Ecoflex 橡胶	波浪结构	碳纳米管	PEDOT/碳纳米管	气相聚合	82 F/g, 11 mF/cm² @10 mV/s	600	600%双向拉伸应变下保持94%电容	[92]
PEDOT:PSS	螺旋结构	PEDOT-S:PSS	PEDOT-S:PSS	湿法纺丝	93.1 mF/cm² @50 μA/cm²	400	400%应变下保持80%电容	[93]
弹性橡胶纤维	螺旋结构	金@碳纳米管	聚苯胺/碳纳米管	电沉积	6 F/cm³@70 A/cm³	400	应变从0%增加到400%保持96%电容	[94]
弹性纤维	螺旋结构	碳纳米管纤维	MnO₂@PEDOT:PSS@碳纳米管	涂覆和电沉积	278.6 mF/cm²	100	100%应变下拉伸循环3000次后保持92%电容	[95]
弹性纤维	螺旋结构	碳纳米管	碳纳米管	包裹	0.515 Wh/kg@ 0.05 A/g	100	75%应变下拉伸循环100次后保持95%电容	[55]
橡胶纤维	螺旋结构	碳纳米管片	MnO₂/碳纳米管	包裹	4.8 mF/cm, 22.8 mF/cm²	40—800	600%应变下保持92.6%电容	[96]
聚合物基底	波浪结构	石墨烯机织布	聚苯胺/ 石墨烯	原位电沉积	17 μF/cm² @0.06 V/s	30	拉伸循环100次后CV 曲线略有下降(应变速率 60%/s)	[97]
橡皮筋	波浪结构	碳纳米管膜	碳纳米管/ 聚苯胺	电沉积	394 F/g@2 mV/s	100	100%应变下拉伸循环100次后保持98%电容	[79]

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可拉伸超级电容器的研究进展:电极、电解质和器件