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Frontiers in Energy

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ISSN 2095-1698(Online)

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Front. Energy    2024, Vol. 18 Issue (5) : 612-639    https://doi.org/10.1007/s11708-024-0911-2
Application and structure of carbon nanotube and graphene-based flexible electrode materials and assembly modes of flexible lithium-ion batteries toward different functions
Yanzhi Cai1(), Zhongyi Hu1, Laifei Cheng2, Siyu Guo1, Tingting Liu1, Shaohua Huang1, Dengpeng Chen1, Yuhan Wang1, Haiming Yu1, Yuan Zhou1
1. College of Materials Science and Engineering, Xi’an University of Architecture and Technology, Xi’an 710055, China
2. Science and Technology on Thermostructure Composite Materials Laboratory, Northwestern Polytechnical University, Xi’an 710072, China
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Abstract

In recent years, the rapid development of portable/wearable electronics has created an urgent need for the development of flexible energy storage devices. Flexible lithium-ion batteries (FLIBs) have emerged as the most attractive and versatile flexible electronic storage devices available. Carbon nanotubes (CNTs) are hollow-structured tubular nanomaterials with high electrical conductivity, large specific surface area, and excellent mechanical properties. Graphene (G) is to some extent comparable to CNTs, because both have unlimited value in flexible electrodes. Herein, a systematic summary of the application of CNT and G in FLIBs electrodes is presented, including different functional applications and services at different temperatures. Furthermore, the effects of electrode structures, including powder, wire-shaped, and film-shaped structures, on electrochemical properties is highlighted. The assembly structures of the FLIBs consisting of CNT and G-based flexible electrodes to realize different functions, including bendability, stretchability, foldability, self-healing, and self-detecting, are systematically reviewed. The current challenges and development prospects of flexible CNT and G-based flexible electrodes and corresponding FLIBs are discussed.
Keywords flexible lithium-ion batteries (FLIBs)      carbon nanotubes (CNTs)      graphene (G)      electrode structure      function     
Corresponding Author(s): Yanzhi Cai   
Online First Date: 05 January 2024    Issue Date: 16 October 2024
 Cite this article:   
Yanzhi Cai,Zhongyi Hu,Laifei Cheng, et al. Application and structure of carbon nanotube and graphene-based flexible electrode materials and assembly modes of flexible lithium-ion batteries toward different functions[J]. Front. Energy, 2024, 18(5): 612-639.
 URL:  
https://academic.hep.com.cn/fie/EN/10.1007/s11708-024-0911-2
https://academic.hep.com.cn/fie/EN/Y2024/V18/I5/612
Fig.1  Application of CNT and G to FLIBs electrodes.
Fig.2  
FunctionalMaterialsMechanical propertyElectrochemical performanceRef.
Conductive agentFe3O4/CNTsTs is 75.2 MPa, E is 73 MPa950 mAh/g (1 A/g)Cheng et al. [64]
SWCNT-GFCurl953 mAh/g (0.1 A/g)Ren et al. [66]
CNF/CNTsBend 0°, 45°, 90°, 135°, 180°1099.5 mAh/g (0.05 A/g)Huang et al. [65]
Flexible skeletonLiNi0.5Mn1.5O4/MWCNTsAt 1.6 cm bending radiusMore than 80% capacity at 20 CFang et al. [126]
LMO/CNTStretch 1000 times97 mAh/g (1 C)Gu et al. [113]
PDI/SWCNTBend 0° to 180°More than 2000 cyclesYang et al. [127]
PMTA//SWCNT@SWCNTBend 1000 times163 mAh/g (200 °C)Wu et al. [129]
G@CNT@MoS2Bend 180°606 mAh/g (200 cycles, 0.2 A/g)Ren et al. [72]
C/meso-Si/CNTsCompress1700 mAh/g (4 A/g)Yang et al. [75]
Active materialSACNTE and Ts are increased by about 10 timesWeight energy density is increased by more than 180%Wang et al. [131]
VACNTs-Si/CCFolded3.33 mAh/cm2Wang et al. [82]
SGCBend1118.2 mAh/g (0.1 A/g)Zhang et al. [85]
Tab.1  Functional applications of CNT/G in flexible FLIB electrode materials
Fig.3  Nuclear shell electrode materials and flexible display.
Fig.4  Yarn line electrode.
Fig.5  Film structure design and flexible display.
Material/filmCathode/anodeElectrochemical performanceMechanical propertyMicrostructureRef.
Si/rGOAnode650 mAh/g(200 mA/g, 150 cycles)CrimpLamellarZhang et al. [102]
GF/SiAnode1.4 mAh/cm2(0.22 mA/cm2)0.95 mAh/cm2 (0.45 mA/cm2)BendableFoamLi et al. [145]
NC/SCAnode1047 mAh/g(0.1 A/g)Bend 0°, 90°, 180°, and foldCamelliaGuo et al. [149]
SiOx/CNTsAnode1240 mAh/g(100 mA/g)441 mAh/g (2 A/g)Folding and rollingSliceGuo et al. [146]
PVDF/SiOx/CNTsAnode820 mAh/g(500 mA/g, 150 cycles)BendingPorousKang et al. [147]
Si/CNTsAnode1400 mAh/g(200 mA/g)Bend and twistLamellarFu et al. [148]
Si/CNTsAnode10.6 mAh/cm2(0.06 mA/cm2)Ts =3.75 MPaNetworkXie et al. [99]
CNTs/(Fe@Si@SiO2)Anode968 mAh/g(1 A/g)Maximum tensile rate 18% (500 g)Core plasma skinZhang et al. [103]
G-PZCOAnode322 mAh/g(8 A/g)Repeated bendingLamellarCao et al. [150]
CA?CNTsCathode5.4 mAh/cm2Repeated bendingLamellarHan et al. [151]
TiO2/G/PVDFAnode165 mAh/g(60 mA/g, 40 cycles)Roll upStackedRen et al. [93]
G/SnO2Anode740 mAh/gBend 180°, 360°, 720°LamellarShang et al. [94]
SWCNTs/PPsCathode106 mAh/g (10 C)BendFiber microporousWang et al. [96]
SWCNTs/SnO2Anode906 mAh/g (200 mA/g)Bend 180°NetworkNoerochim et al. [152]
SnO2-G(SGN)Anode540 mAh/g (1 C)BendableSheetWang et al. [98]
CNF/CNTs@ EGaIn NPsAnode420 mAh/g (800 mA/g, 100 cycles)BendableFibrous networkYu et al. [101]
BSGAnode203 mAh/g (50 mA/g, 100 cycles)BendableLamellarChen et al. [153]
pMn3O4 NR/rGOAnode618 mAh/g (100 mA/g)BendableSheetPark et al. [154]
NCMTs@A-MoS2/rGOAnode544 mAh/g(1 A/g, 1000 cycles)FoldableTubular networkLiu et al. [155]
Tab.2  Mechanical and electrochemical properties of CNT/G-based film electrode materials
Fig.6  Battery assembly and multifunctional.
Fig.7  Assembly and mechanical properties of FLIB.
Fig.8  Self-healing and wrist band battery.
Different functionsStructureMechanicalElectrochemical propertiesRef.
BendabilitySandwichKeeping LED light dark for 30 min0.5 mA/cm2 (2.6 mAh/cm2)Zhong et al. [112]
PlanarityBending to 6 mmEnergy density of 108 MWh/gHu et al. [105]
PlanarityBending 300°0.2 C (126 mAh/g)Aliahmad et al. [104]
Coaxial fiberBending knotVolume energy density of 144.82 MW/cm3Song et al. [109]
FiberBending 90°Energy density of 30.12 Wh/kgZhang et al. [111]
Coaxial fiberAble to be wovenWeight density of 27.7 MWh/gWeng et al. [110]
StretchabilityHelical9000 stretching cyclesEnergy density of 4.862 mAh/cm3Kammoun et al. [158]
Spring-like200 100% stretching cyclesEnergy density of 27 Wh/kg;Power density of 880 W/kgRen et al. [115]
Fibrous100% strainCapacity retention rate of 85%Zhang et al. [138]
FoldabilityPlanarityFold and release LED for continuous lightExtend service lifeLiu et al. [116]
PlanarityNo significant change in the light emission of the 5-fold LED0.2 C (164.3 mAh/g)Hu et al. [159]
Planarity500 foldsWeight energy density of 252 Wh/kgVolume energy density of 332.05 Wh/LMu et al. [118]
PlanarityStill able to power the LED after foldingCapacity of 138.3 mAh/gWei et al. [117]
Self-healing abilityPlanarityReconstruction of H bond after cuttingEnergy density of 32.04 Wh/kgZhao et al. [165]
PlanarityReconstruction of H bond is after cutting0.1 A/g (5 times healing, capacity of 50.1 mAh/g)Rao et al. [166]
Self-detecting abilityPlanarityBend, twist, foldDetect heart rate;Resource sustainabilityKuznetsov et al. [167]
Tab.3  FLIBs with different structures and functions
Fig.9  Prospects of CNT and G-based FLIBs.
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