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Reevaluating Flexible Lithium-Ion Batteries from the Insights of Mechanics and Electrochemistry

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Abstract

The emerging direction toward the ever-growing market of wearable electronics has contributed to the progress made in energy storage systems that are flexible while maintaining their electrochemical performance. Endowing lithium-ion batteries with high flexibility is currently considered to be one of the most essential choices in future. Here, we first propose the basic deformation mode according to the manifestation of flexibility and constructively reevaluate the concept of flexible lithium-ion batteries. Furthermore, the failure mechanism of flexible lithium-ion batteries is investigated with regard to their mechanical failure and electrochemical failure, and the related strategies of battery design and manufacturing are analyzed. More importantly, an in-depth analysis is conducted on the approaches to overcome mechanical failure through stress dispersion, stress absorption, prestress concentration, stress transfer, and other flexible reinforcement methods. Additionally, the advantages of suppressing electrochemical failure are discussed by enhancing the surface roughness, pore formation, surface coating, chemical bonding, in situ encapsulation, etc. Regarding self-healing technology, the general approaches taken for self-healing batteries to achieve flexibility are explained through the classification of macroscopic self-healing (to avert mechanical failure) and microscopic self-healing (to respond to electrochemical failure). Finally, after considering the current state of flexible lithium-ion batteries, future challenges are presented.

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The flexible lithium-ion batteries were re-evaluated from the insights of mechanics and electrochemistry.

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Fig. 1
Fig. 2

Copyright 2014, Nature Publishing Group. d Foldable patterns are designed with three topologies. Reprinted with permission from Ref. [49]. Copyright 2015, Nature Publishing Group. e Optical images of edge-cut and center-cut kirigami cathodes in bent, twisted, and stretched states. f Illustration of the electrode microstructure. g Simulation results of electrode strain by FEA. h Kirigami LIBs light up an LED in static and stretched states. Reprinted with permission from Ref. [50]. Copyright 2020, American Chemical Society

Fig. 3

Copyright 2017, Wiley–VCH. d Schematic of the structure and fabrication process of spine-like integrated FLIBs. e Simulation results of battery strain by FEA. Reprinted with permission from Ref. [52]. Copyright 2018, Wiley–VCH. f Fabrication process and g schematic diagram of the accordion-like integrated FLIB structure. h Stress contours of the stretchable layers without (left) and with (right) tape protection. SEM images of the i unprotected and j protected electrodes after stretching. Reprinted with permission from Ref. [53]. Copyright 2019, Elsevier

Fig. 4

Copyright 2021, Royal Society of Chemistry. i Snake-origami batteries and their structural parameters. j, k Different types of snake-origami batteries with bidirectional deformation. Reprinted with permission from Ref. [54]. Copyright 2021, Wiley–VCH. l Internal structure of sawtooth-like FLIBs and m digital photographs. n Schematic of a battery in a bent state. o Changes in the open-circuit voltage as a function of the number of bending cycles. Reprinted with permission from Ref. [55]. Copyright 2017, Wiley–VCH

Fig. 5

Copyright © 2015, American Chemical Society

Fig. 6

Copyright 2009, American Chemical Society. b SEM image of a flexible cellulose/graphite paper electrode. Reprinted with permission from Ref. [58]. Copyright 2012, Royal Society of Chemistry. c Micropores and cracks on the surface of graphene film and d its rate performance. Reprinted with permission from Ref. [59]. Copyright 2012, American Chemical Society. e SEM and f TEM images of a highly porous CNF. Reprinted with permission from Ref. [60]. Copyright 2015, Elsevier. g Relative flexibility of the porous structure as a function of porosity. Reprinted with permission from Ref. [62]. Copyright 2019, American Chemical Society. h Graded structure of bamboo. i Schematic of the bamboo-inspired nanostructure design. j TEM image of a bamboo-like CNF. k Results from three-point bending simulations of different fiber geometries. Reprinted with permission from Ref. [63]. Copyright 2015, American Chemical Society

Fig. 7

Copyright 2014, Wiley–VCH. c SEM images (top view) of patterned Al (left) and Cu (right) foils. d Cycle capacity of the battery. Reprinted with permission from Ref. [66]. Copyright 2014, American Chemical Society. e Fabrication process and f surface topography of the patterned current collector. g Plot of the surface coverage of electrodes versus the bending/twisting cycle. Reprinted with permission from Ref. [67]. Copyright 2014, Wiley–VCH. h Schematic of the 3D interlocking full cell. Adhesion force curves of the i LCO cathode and j graphite anode. k Voltage profiles of 5 000 flexing cycles for 40 h at the fully charged state of the unstressed, normal, and 3D interlocking full cell. Reprinted with permission from Ref. [68]. Copyright 2018, Wiley–VCH

Fig. 8

Copyright 2019, Elsevier. d Surface stress on curved electrode structures. Illustration of the e structural damage of an electrode and f vertical array of an electrode surface. g Synthesis process of the in situ growth of L-LCO nanosheet arrays. h, i FESEM images of the L-LCO nanosheet arrays. j Cycling performance of a full cell. k Discharge curves of the nanosheet-based full cell. Reprinted with permission from Ref. [88]. Copyright 2018, Wiley–VCH

Fig. 9

Copyright 2018, Royal Society of Chemistry. b Preparation process and c cycling stability of bendable coaxial fiber LIBs. Reprinted with permission from Ref. [92]. Copyright 2014, American Chemical Society. d Schematic diagram and side-view photograph of a bendable coaxial cable LIB. Reprinted with permission from Ref. [93]. Copyright 2018, Wiley–VCH. e Schematic illustration of a twisted structure. Reprinted with permission from Ref. [90]. Copyright 2018, Royal Society of Chemistry. f Schematic illustration of a wire-shaped LIB fabricated by twisting an aligned MWCNT/MnO2 composite fiber and Li wire as positive and negative electrodes, respectively. The inserted top left image shows the charge–discharge process. Reprinted with permission from Ref. [94]. Copyright 2013, Wiley–VCH. g Schematic illustration of a half LIB based on an aligned MWCNT/Si composite fiber as the working electrode and lithium wire as both the counter and reference electrodes. Reprinted with permission from Ref. [95]. Copyright 2014, Wiley–VCH. h Structure of a flexible wire-shaped LIB. The aligned MWCNT/LTO and MWCNT/LMO composite yarns are paired as the anode and cathode, respectively. Reprinted with permission from Ref. [96]. Copyright 2014, Wiley–VCH. i Fabrication process illustration and j photographs of a super-stretchy LIB. Reprinted with permission from Ref. [98]. Copyright 2014, Royal Society of Chemistry. k SEM images of fiber at different strains. Reprinted with permission from Ref. [99]. Copyright 2014, Wiley–VCH. l–o 1D battery being woven into a textile. Reprinted with permission from Ref. [92]. Copyright 2014, American Chemical Society. Reprinted with permission from Ref. [96]. Copyright 2014, Wiley–VCH. Reprinted with permission from Ref. [98]. Copyright 2014, Royal Society of Chemistry. Reprinted with permission from Ref. [101]. Copyright 2016, Royal Society of Chemistry

Fig. 10

Copyright 2017, Wiley–VCH. e SEM image of MoSe2/SWCNT. f C K-edge X-ray absorption near-edge structures. g Schematic illustration and h rate performance of a 1 T-MoSe2/SWCNT electrode. Reprinted with permission from Ref. [103]. Copyright 2017, American Chemical Society. The SEM images of the electrode were derived from i ZIF-67@PAN and j MIL-88@PAN. k Cycling stability of ZIF-67@PAN, MIL-88@PAN, and PAN electrodes. Reprinted with permission from Ref. [104]. Copyright 2018, Wiley–VCH. l Schematic diagram of a single nanocable where V2O5 is uniformly encapsulated in a graphitic nanotube. m TEM image of V2O5@CNT. n Cycling life and o rate performance of V2O5@CNT. Reprinted with permission from Ref. [105]. Copyright 2016, Royal Society of Chemistry

Fig. 11

Copyright 2017, Wiley–VCH. Schematic diagram of the c flexible substrate/active material/flexible substrate structure and d active material/flexible/active material structure. Reprinted with permission from Ref. [108]. Copyright 2016, Royal Society of Chemistry. Reprinted with permission from Ref. [107]. Copyright 2019, American Chemical Society. e Schematic illustration of the assembly of hierarchical chiral architectures and the fabrication of a flexible SnO2/CNC/rGO film and fiber electrodes with hierarchical chiral structures. f, g Polarized optical microscopy images of GO and CNCs. h 3D AFM image and i small-angle X-ray scattering (SAXS) pattern of CNC/GO. j Cycling performance and k stress–strain curves of samples. Reprinted with permission from Ref. [109]. Copyright 2017, Royal Society of Chemistry

Fig. 12

Copyright 2015, Wiley–VCH. Enlarged views of the wavy structure e before and f after 1 000 stretching cycles at a strain of 400%. g Schematic showing the fabrication of a stretchable CNT electrode. h SEM images of CNT/LTO. i Normalized resistance changes of prestrained CNT/LTO and CNT/NCM electrodes on different axes. j Illuminated LED powered by stretchable NCM/LTO batteries with strain along both the X and Y axes. Reprinted with permission from Ref. [115]. Copyright 2018, Royal Society of Chemistry

Fig. 13

Copyright 2013, Nature Publishing Group. e Schematic illustration of a spin-coating procedure to assemble a film battery. f Stacked film layer battery configuration of the anode–SiO2–MPE–cathode layers. g Conductivity of the film at various geometrical states. h Charge–discharge capacities as a function of the cycle number for the integrated full cell model. Reprinted with permission from Ref. [124]. Copyright 2019, Wiley–VCH

Fig. 14

Copyright 2016, Wiley–VCH. e Schematic illustration of the PVA/PA gel self-healing mechanism. f Stress–strain curves of the obtained gel. Reprinted with permission from Ref. [131]. Copyright 2019, Elsevier. g Illustration showing the formation of dynamic borate ester bonding between SH chains. h Optical image of a twisted SIB. i Cycling characteristics and Nyquist plots of a battery. Reprinted with permission from Ref. [132]. Copyright 2019, American Chemical Society

Fig. 15

Copyright 2013, Nature Publishing Group. c Electrode design toward tuning the spatial distribution of self-healing polymer (SHP)/carbon black in the Si layer. Reprinted with permission from Ref. [134]. Copyright 2015, Wiley–VCH. d Synthesis procedure of an rGO/CNT-supported liquid metal nanoparticle anode. e–g Morphological changes of the electrode surface. h EIS tests of the battery before and after cycling. Reprinted with permission from Ref. [135]. Copyright 2017, Royal Society of Chemistry. i In situ TEM press experiment of a yolk-shell Si@TiO2 nanocluster. j Schematic illustrations of the self-healing mechanism. k Cycling life and corresponding Coulombic efficiency. Reprinted with permission from Ref. [136]. Copyright 2017, Royal Society of Chemistry

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21905071, 21773049), China Postdoctoral Science Foundation (2021T140158, 2018M640298), and Heilongjiang Postdoctoral Fund (LBH-TZ2010, LBH-Z18065).

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  1. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, Heilongjiang, China

    Qi Meng, Shuaifeng Lou, Baicheng Shen, Xin Wan, Xiangjun Xiao, Yulin Ma, Hua Huo & Geping Yin

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QM wrote this paper. BS, XW, and XX conducted the literature survey. YM and HH provided writing guidance. SL and GY supervised all the processes and provided financial support.

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Meng, Q., Lou, S., Shen, B. et al. Reevaluating Flexible Lithium-Ion Batteries from the Insights of Mechanics and Electrochemistry. Electrochem. Energy Rev. 5 (Suppl 2), 30 (2022). https://doi.org/10.1007/s41918-022-00150-w

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