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复合材料结构超级电容器碳纤维电极的制备与改性方法研究进展

陈少杰,  徐海兵,  张雪辉,  刘东,  颜春,  陈刚,  吕东喜,  祝颖丹

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文章导航 > 复合材料学报  > 2023 >  40(11): 6010-6028
陈少杰, 徐海兵, 张雪辉, 等. 复合材料结构超级电容器碳纤维电极的制备与改性方法研究进展[J]. 复合材料学报, 2023, 40(11): 6010-6028. doi: 10.13801/j.cnki.fhclxb.20230601.001
引用本文: 陈少杰, 徐海兵, 张雪辉, 等. 复合材料结构超级电容器碳纤维电极的制备与改性方法研究进展[J]. 复合材料学报, 2023, 40(11): 6010-6028. doi: 10.13801/j.cnki.fhclxb.20230601.001
shu
CHEN Shaojie, XU Haibing, ZHANG Xuehui, et al. Recent progress in carbon fiber electrodes for structural supercapacitors composites[J]. Acta Materiae Compositae Sinica, 2023, 40(11): 6010-6028. doi: 10.13801/j.cnki.fhclxb.20230601.001
Citation: CHEN Shaojie, XU Haibing, ZHANG Xuehui, et al. Recent progress in carbon fiber electrodes for structural supercapacitors composites[J]. Acta Materiae Compositae Sinica, 2023, 40(11): 6010-6028. doi: 10.13801/j.cnki.fhclxb.20230601.001
shu

复合材料结构超级电容器碳纤维电极的制备与改性方法研究进展

doi: 10.13801/j.cnki.fhclxb.20230601.001
  • 1.

    江西理工大学　材料冶金化学学部，赣州 341000

  • 2.

    中国科学院宁波材料技术与工程研究所 浙江省机器人与智能制造装备技术重点实验室，宁波 315201

基金项目: 国家自然科学基金(U1909220)；浙江省自然科学基金(LY21E030012)；宁波市科技创新2025重大专项(2019B10112；2020Z057；2021Z126；2022Z102)
详细信息
    通讯作者:

    徐海兵，博士，副研究员，硕士生导师，研究方向为碳纤维复合材料　E-mail：xuhaibing@nimte.ac.cn；

    张雪辉，博士，副教授，硕士生导师，研究方向为铜基复合材料　E-mail：xhzhang@jxust.edu.cn

  • 中图分类号: TB332

Recent progress in carbon fiber electrodes for structural supercapacitors composites

  • 1.

    Faculty of Material Metallurgy and Chemistry, Jiangxi University of Science and Technology, Ganzhou 341000, China

  • 2.

    Zhejiang Provincial Key Laboratory of Robotics and Intelligent Manufacturing Equipment Technology, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China

Funds: National Natural Science Foundation of China (U1909220); Natural Science Foundation of Zhejiang Province (LY21E030012); Ningbo Key Projects of Science and Technology Innovation 2025 Plan (2019B10112; 2020Z057; 2021Z126; 2022Z102)

    摘要
  • 摘要: 在能源危机与生态环境持续恶化的大背景下，开发先进储能技术成为各国竞相研究的重点。将碳纤维作为多功能结构电极与聚合物电解质复合，制备兼具储能与结构承载的复合材料结构超级电容器(Structural supercapacitor composites，SSC)，有望满足现代装备对高效储能与轻量化结构的双重需求，在新能源汽车、航空航天等领域具有广泛应用前景。碳纤维电极是SSC的重要组件，承担着富集电荷与力学承载的双重任务，应具有高比表面积、优良的力学性能及树脂电解质浸润能力。然而常规碳纤维表面光滑，比表面积小，化学惰性大，不利于电荷的存储及树脂电解质的浸润，限制了高性能SSC的制备与应用，必须对其进行表面改性处理。本文介绍了SSC用碳纤维电极材料的研究现状，重点阐述了刻蚀活化改性、碳基活性材料修饰、纳米金属化合物活性材料修饰、聚苯胺修饰等改性方法，总结了不同碳纤维电极制备方法对SSC储能及力学性能的影响行为与机制，归纳了各自优缺点，并展望了SSC用碳纤维电极研制面临的挑战及发展趋势。

     

    Abstract: In the context of energy crisis and continuous deterioration of ecological environment, the development of advanced energy storage technology has become the focus of competing research in global. Structural supercapacitor composites (SSC) with both energy storage and structural bearing capacity are developed by using multifunctional carbon fiber electrode and polymer electrolyte, which is expected to meet the dual demands of modern equipment for efficient energy storage and lightweight structures. Therefore, SSC has a wide application prospect in electric vehicles, aerospace and other fields. Carbon fiber electrode is a key component of SSC, which plays an important role in charge accumulation and mechanical loading. It should have high specific surface area, excellent mechanical properties and good wettability with polymer electrolyte. However, the pristine surface of carbon fiber is smooth and chemically inert, which is not conducive to ion storage and resin electrolyte infiltration in carbon fiber electrodes, and thus limits the preparation and application of high-performance SSC, so surface modification of carbon fiber electrode is necessary. This paper introduces the current research status of carbon fiber electrode materials for SSC, mainly focuses on several important surface modification methods of carbon fiber (such as chemical etching activation, modification with carbon-based active materials, modification with nano metal compounds and polyaniline modification), summarizes the influence of different carbon fiber electrode preparation methods on the energy storage and mechanical properties of SSC and the corresponding mechanisms, and their respective advantages and disadvantages. The challenges and development trend of carbon fiber electrode for SSC are also prospected.

     

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  • 图  1  超级电容器储能原理示意图及电极材料示意图：(a) 双电电容器；(b) 赝电容电容器[8]

    Figure  1.  Schematic illustration of supercapacitor energy storage principle and its electrode material: (a) Electric double layer capacitors; (b) Pseudocapacitor capacitors[8]

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    图  2  电介质电容器、电池、燃料电池和超级电容器的Ragone图[9]

    Figure  2.  Ragone plots for representative energy storage devices of dielectric capacitors, batteries, fuel cells and supercapacitors[9]

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    图  3  复合材料结构超级电容器及其储能原理示意图

    Figure  3.  Schematic illustration of structural supercapacitor composites and its principle of energy storage

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    图  4  热空气活性碳纤维布的过程示意图[21]

    CFCs—Carbon fiber cloth

    Figure  4.  Schematic for the preparation process of activated carbon fiber cloths[21]

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    图  5  SEM微观形貌：((a), (b))未活化的碳纤维；((c), (d)) KOH热刻蚀活化的碳纤维[22]

    Figure  5.  SEM images: ((a), (b)) As-received carbon fibre; ((c), (d)) KOH activated carbon fibre[22]

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    图  6  SEM微观形貌：((a), (b))未改性的碳纤维；((c), (d)) HNO3化学-热氧活化协同处理的碳纤维[24]

    Figure  6.  SEM images: ((a), (b)) As-received carbon fibre; ((c), (d)) Activated carbon fibre by HNO3 and thermally oxidization[24]

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    图  7  基于活性碳修饰碳纤维电极的复合材料结构超级电容器(SSC)制备工艺示意图[18]

    C—Conductive agent; AC—Activated carbon; WCF—Carbon fiber woven cloth; PTEE—Polytetrafluroethylene

    Figure  7.  Schematic for the preparation of structural supercapacitor composite (SSC) based on activated-carbon-coated carbon fiber electrodes[18]

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    图  8  基于喷涂工艺制备石墨烯纳米片(GNP)修饰碳纤维布电极的示意图[27]

    Figure  8.  Schematics for the preparation of graphene nanoplatelet (GNP) modified carbon fiber woven cloth electrode based on spraying process[27]

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    图  9  碳纤维电泳沉积(EPD)连续沉积石墨烯工艺的示意图[27]

    Figure  9.  Schematic for the fibre treatment line for continuous electrophoretic deposition (EPD) on carbon fibres[27]

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    图  10  基于连续EPD技术得到的石墨烯纳米片修饰碳纤维的表面特征形貌：(a) 30 V条件下沉积1 min；(b) 40 V条件下沉积1 min[27]

    Figure  10.  Characteristic micrographs of graphene nanoplatelet coated carbon fibres produced using the continuous EPD process at the following conditions: (a) 30 V, 1 min; (b) 40 V, 1 min[27]

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    图  11  SSC制备过程示意图：(a) CF → gCF ： 等离子体强化气相沉积技术(rf-PECVD)在裸碳纤维布上生长石墨烯纳米片(GNFs)；(b) gCF → UgCF：通过尿素活化石墨烯纳米片沉积过的碳纤维布；(c) CF–(2GFs:SPE)–CF叠放的多功能结构超级电容器(MSS)结构示意图；(d)树脂灌注法制备碳纤维增强聚合物(CFRP)复合材料 MSS 层压板[29]

    PEGDGE—Polyethylene glycol diglycidyl ether; IL—Ionic liquid; TETA—Triethylene-tetramine; GFs—Glass fabrics

    Figure  11.  Schematic illustration of steps used for the fabrication of structural supercapacitor: (a) CF → gCF : direct growth of graphene nanoflakes (GNFs) on bare carbon fiber (CF) fabrics by plasma enhanced vapor deposition technique (rf-PECVD); (b) gCF → UgCF : urea activation of GNFs-coated carbon fiber ( gCF ) fabrics ( UgCF ); (c) CF–(2GFs:SPE)–CF lay-up configuration of multifunctional structural supercapacitor (MSS); (d) Fabrication of carbon fiber reinforced polymer (CFRP) composite-based MSS laminates via the resin infusion method[29]

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    图  12  SEM微观形貌：(a) 未改性的碳纤维电极；(b) 多壁碳纳米管(MWCNT)修饰的碳纤维电极[30]

    Figure  12.  SEM images: (a) As-received carbon fibre; (b) Carbon fibre modified by multi-walled carbon nanotubes (MWCNT)[30]

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    图  13  不同MWCNT负载量与改性碳纤维比电容的关系(比电容通过测试扫速为1 mV/s、10 mV/s、100 mV/s的CV曲线计算得到)[14]

    Figure  13.  Specific capacitance of MWCNT-impregnated carbon fiber electrodes as increasing amounts of MWCNT measured with CV experiments at 1 mV/s, 10 mV/s and 100 mV/s[14]

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    图  14  基于碳气凝胶修饰的碳纤维结构电极制备SSC示意[17]

    Figure  14.  Schematic for the prepration of SSC based on carbon aerogel modified carbon fiber structured electrode[17]

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    图  15  SEM微观形貌：(a) 初始碳纤维；((b)~(d)) 碳气凝胶修饰的碳纤维[17]

    Figure  15.  SEM images: (a) As-received carbon fiber; ((b)-(d)) Carbon fiber modified by carbon aerogel[17]

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    图  16  通过负载石墨烯气凝胶制备碳纤维结构电极的示意图[19]

    GA—Graphene aerogel; GO—Graphene oxide

    Figure  16.  Schematic for the preparation of carbon fiber structured electrode by loading graphene aerogel[19]

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    图  17  不同水热反应时间下MnOOH的微结构形貌[33]

    Figure  17.  SEM images of MnOOH obtained under different hydrothermal reaction time[33]

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    图  18  基于MnOOH-NWs@WCF电极制备SSC的示意图[33]

    NWs—Nanowires; WCF—Carbon fiber woven cloth; GFF—Glass fibre fabric

    Figure  18.  Schematic for the preparation of SSC based on MnOOH-NWs@WCF electrode[33]

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    图  19  (a) ZnO纳米棒修饰WCF的表面微观形貌；((b)~(f)) 在0.18 mol/L KOH水溶液刻蚀2 h、4 h、5 h、5.5 h、6 h得到的ZnO纳米管修饰WCF的微观形貌[34]

    Figure  19.  (a) Surface micromorphology of ZnO nanorods/WCF; ((b)-(f)) Surface micromorphology of ZnO nanotubes/WCF obtained by etching in 0.18 mol/L KOH aqueous solution for different time (2 h, 4 h, 5 h, 5.5 h and 6 h)[34]

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    图  20  VG/MnO2改性碳布电极制备过程及其相应的SSC组成示意图[12]

    PECVD—Plasma enhanced chemical vapor deposition; VG—Vertical graphene; ECD—Electrochemical deposition

    Figure  20.  Schematic for the preparation of VG/MnO2 modified carbon fiber electrode and the corresponding SSC[12]

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    图  21  不同放大倍数下包覆碳层的Ni-Co氧化物纳米线(CCNC Nws)@WCF电极微结构形貌[40]

    Figure  21.  SEM images of carbon-coated Ni-Co core-shell nanowires (CCNC Nws)@WCF electrode under different magnification[40]

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    图  22  微观形貌：(a) 原始碳纤维；(b) 活化碳纤维；(c) 碳布(CF)-PANI-0.05纤维；(d) 活化碳布(ACF)-APNI-0.05纤维[42]

    PANI—Polyaniline

    Figure  22.  Microstructure: (a) As-received carbon fiber; (b) Activated carbon fiber; (c) Carbon fibre(CF)-PANI-0.05 fiber; (d) Activated carbon fibre (ACF)-APNI-0.05 fiber[42]

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    图  23  碳纤维电极改性方法及其结构超级电容器组装示意图

    Figure  23.  Schematic diagram of the modification method of carbon fiber electrode and assembly of its structural supercapacitor

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    表  1  未改性碳纤维与活化改性碳纤维的比表面积与拉伸强度[22]

    Table  1.   Specific surface area and tensile strength of as-received and activated carbon fibre[22]

    SampleSpecific surface
    area/
    (m2·g-1)    		Tensile strength/
    MPa
    As-received 0.213300±200
    HNO3 activated 0.503100±260
    Air activated 0.601900±220
    CO2 activated 1.102400±250
    KOH activated23.303600±320
    下载: 导出CSV

    表  2  不同改性碳纤维电极的比表面积与比电容[17]

    Table  2.   Surface area and specific capacitance of carbon fiber electrodes by different modification[17]

    SampleCAG loading/wt%BET surface area/(m2·g−1)Specific capacitance/
    (F·g−1)
    As-received– 0.21 0.06
    CAG-modified
    (press)    		22.0163.1014.30
    CAG-modified
    (infusion)    		15.9118.00 8.70
    CAG-modified
    (infusion)    		 9.5 80.70 5.90
    Notes: CAG—Carbon aerogels; BET—Brunauer-Emmett-Teller.
    下载: 导出CSV

    表  3  不同改性碳纤维电极的性能对比

    Table  3.   Performance comparison of different modified carbon fiber electrodes

    电极材料电解质比电容力学性能文献
    ACFPC/PEGDGE/TBAPF63.1 F/g (SSC)器件压缩强度：28.81 MPa；
    器件压缩模量：35.08 MPa    		[24]
    WCF/AC15DGEBA/AG-85/EMIMTFSI13.12 F/g (SSC)器件拉伸强度：257.78 MPa；
    器件拉伸模量：23.20 MPa    		[18]
    GNP-WCFTEABF4/PC1.44 F/g (小尺寸SSC)器件拉伸强度：350 MPa；
    器件拉伸模量：26 GPa    		[27]
    623 mF/g (大尺寸SSC)
    CNT-CF1 mol/L KCl3.1 F/g (电极)–[30]
    CD553/SR494/EMITSFI125 mF/g (SSC)–
    ZnO-WCFLSP-8020 B/EMITSFI/LiTf/PANI18.8 F/g (SSC)器件拉伸强度：325.82 MPa；[34]
    Cu-CoSe NWs@WCFLPS-8020 B/EMIMBF4/LiTf28.63 F/g (SSC)器件拉伸强度：488.89 MPa；
    器件拉伸模量：32.65 GPa    		[10]
    CF/VG/MnO21 mol/L Na2SO4240 F/g (电极 )–[12]
    PEGDGE/EMITSFI/LiTFSI)30.7 mF/cm2 (SSC)器件拉伸强度：85.6 MPa
    CF/PANILiClO4/DGEBA/PC20.05 mF/g (SSC)–[42]
    Notes: PEGDGE—Poly(ethylene glycol) diglycidyl ether; TBAPF6—Tetra-n-butylammonium hexafluorophosphate; DGEBA—Digycidylether of bis-phenol-A; EMIMTFSI—1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide; TEABF4—Tetraethylammonium tetrafluoroborate; LiTf—Lithium trifluoromethanesulfonate; EMIMBF4—1-ethyl-3-methylimidazolium tetrafluoroborate; LiTFSI—Lithium bis((trifluoromethyl)sulfonyl)azanide.
    下载: 导出CSV
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  • 收稿日期:  2023-03-01
  • 修回日期:  2023-05-04
  • 录用日期:  2023-05-26
  • 网络出版日期:  2023-06-02
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