Abstract
Replacement of liquid electrolytes with polymer gel electrolytes is recognized as a general and effective way of solving safety problems and achieving high flexibility in wearable batteries1,2,3,4,5,6. However, the poor interface between polymer gel electrolyte and electrode, caused by insufficient wetting, produces much poorer electrochemical properties, especially during the deformation of the battery7,8,9. Here we report a strategy for designing channel structures in electrodes to incorporate polymer gel electrolytes and to form intimate and stable interfaces for high-performance wearable batteries. As a demonstration, multiple electrode fibres were rotated together to form aligned channels, while the surface of each electrode fibre was designed with networked channels. The monomer solution was effectively infiltrated first along the aligned channels and then into the networked channels. The monomers were then polymerized to produce a gel electrolyte and form intimate and stable interfaces with the electrodes. The resulting fibre lithium-ion battery (FLB) showed high electrochemical performances (for example, an energy density of about 128 Wh kg−1). This strategy also enabled the production of FLBs with a high rate of 3,600 m h−1 per winding unit. The continuous FLBs were woven into a 50 cm × 30 cm textile to provide an output capacity of 2,975 mAh. The FLB textiles worked safely under extreme conditions, such as temperatures of −40 °C and 80 °C and a vacuum of −0.08 MPa. The FLBs show promise for applications in firefighting and space exploration.
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Data availability
The data that support the findings of this study are available from the corresponding author upon request. Source data are provided with this paper.
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Acknowledgements
This work was supported by MOST (2022YFA1203001 and 2022YFA1203002), NSFC (T2321003, 22335003, 52122310, 22075050, 52222310, T2222005 and 22175042), STCSM (21511104900) and China Postdoctoral Science Foundation (2023M740651). We thank XPLORER PRIZE for its support in fabricating and studying FLBs.
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Contributions
H.P. conceived and designed the project. C.L., H.J. and X.C. performed the design of the FLB with channels, gel electrolytes and FLB textiles. J.H., Y.L., Y.C. and X.G. performed the fabrication of the FLB. K.Z., J.L., Z.Z., X. Shi, L.Y. and M.L. analysed the data. J. Wu, J. Wang and Y.Z. performed the fabrication of weaving textiles. X. Sun, B.W., P.C. and Y.W. contributed to the discussion on the data, figures and manuscript. C.L., X.C. and H.P. wrote the paper.
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Extended data figures and tables
Extended Data Fig. 1 Electrochemical performances of FLBs deposited with different particle layers.
a,b, Electrochemical impedance spectra and discharge profiles of the FLBs, respectively. The FLBs were discharged at a rate of 0.2C.
Extended Data Fig. 2 Architecture and wetting capability of a fibre electrode with aligned and networked channels.
a, SEM image of a fibre electrode with a rotating architecture. b,c, Magnified SEM images of the aligned fibres and the channel between them, respectively. d,e, Images reconstructed from X-ray computed tomography data of the networked channels (blue) among particles (grey), respectively. The particles were highly interconnected with each other, forming channels among them. The small channels showed sizes of several micrometres, while the large channels showed sizes of tens of micrometres. f, Channel size distribution tested by the mercury intrusion method. g–j, Fluorescence microscopy images showing the monomer solution infiltrating along the aligned channels. k, Monomer solution wetting into the networked channels of an electrode. Scale bars, 1 mm (a); 300 μm (b); 100 μm (c); 20 μm (d,e); and 200 μm (g–j).
Extended Data Fig. 3 Electrochemical characterization of FLBs with and without aligned channels.
a,b, Cyclic voltammograms of the FLBs with and without aligned channels at increasing scan rates, respectively. FLBs without aligned channels showed obvious polarizations at high scan rates. The voltage ranges were set within 50 mV near the open-circuit voltage to obtain capacitance currents. c, Specific capacitances of FLBs with and without aligned channels at increasing scan rates. d, Charge–discharge profiles of FLBs with and without aligned channels. The FLB with aligned channels showed much higher specific capacity because of sufficient wetting by the electrolyte through the aligned channels. The electrolyte amounts were around 8 g/Ah.
Extended Data Fig. 4 Characterization of FLBs with and without an inner small particle layer.
a,b, Cross-sectional SEM images of cathode fibres with and without an inner small particle layer, respectively. c, Charge–discharge profiles of FLBs with and without an inner small particle layer. The FLBs were discharged at a rate of 2C. d,e, Raman shifts of LiCoO2 particles at 5 different positions in the deposition layer of cathode fibre with and without inner small particles, respectively. The cathode fibre with an inner small particle layer showed sufficient lithium ion intercalation after discharging, indicated by the characteristic peaks of the LiCoO2 at 486 cm−1 and 587 cm−1; while the cathode fibre without an inner small particle layer showed insufficient lithium ion intercalation. a.u., arbitrary units. Scale bars, 20 μm (a,b).
Extended Data Fig. 5 Stability of the gel electrolyte–graphite interface.
a–c, Raman mapping images of the gel electrolyte and graphite particles with the FLB in the uncharged state at 3.0 V, half charged state at 3.9 V and a fully charged state at 4.4 V. d,e, Raman mapping images of the gel electrolyte and graphite particles after the FLB was stored at −40 °C and 80 °C for 1 h, respectively. f, Magnified area of the gel electrolyte–graphite interface. g, Corresponding Raman shifts of the graphite particles at 3.0 V, 3.9 V, and 4.4 V. The characteristic peaks of graphite at 1,350 cm−1 and 1,580 cm−1 varied for the different charged states. a.u., arbitrary units. Scale bars, 3 μm (a–e); 1 μm (f).
Extended Data Fig. 6 Architectures and electrochemical properties of FLBs with increasing numbers of electrode fibres.
a–c, SEM images of electrodes with 4, 6, and 8 fibres. The anode fibres were wrapped with separators to prevent short circuits before rotated with the cathode fibres. d, Discharge profiles of FLBs made with increasing numbers of electrode fibres. e, Specific capacities of the FLBs made with increasing numbers of electrode fibres. Error bars show the standard deviations for the results from three samples. Scale bars, 1 mm (a–c).
Extended Data Fig. 7 Charge–discharge performances of different fibre electrodes and LiCoO2//graphite FLBs with different electrolytes.
Charge–discharge profiles of the fibre electrodes of the anode materials of mesocarbon microbeads (MCMB) (a), hard carbon (b), silicon carbon composites (SiC) (c), and Li4Ti5O12 (LTO) (d). Charge–discharge profiles of the fibre electrodes of the cathode materials of LiNi0.5Co0.2Mn0.3O2 (NCM523) (e) and LiMn2O4 (LMO) (f). From a to f, lithium metal was used as the counter electrode, and poly(ethylene glycol) dimethacrylate monomer was used to prepare the gel electrolyte. Charge–discharge profiles of LiCoO2//graphite FLBs were based on the gel electrolytes prepared from different monomers of tri(propylene glycol) diacrylate (TPGDA) (g), pentaerythritol tetraacrylate (PETEA) (h), 1,6-hexanediol dimethacrylate (HADMA) (i), poly(ethylene glycol) diacrylate (PEGDA) (j), and trimethylolpropane triacrylate (TPTEA) (k). l, Initial Coulombic efficiencies of FLBs with different gel electrolytes polymerized from monomers from g to k.
Extended Data Fig. 8 Electrochemical stabilities of the FLB at different temperatures and after immersion in water.
a, FLBs charged at 25 °C at 0.2C and discharged at 0.1C, 0.2C and 0.5C at 0 °C, 25 °C and 80 °C, respectively. b, The FLB charged at 25 °C at 0.2C and discharged at −40 °C at 0.1C with a cut-off voltage of 2 V. c, Capacity retention of the FLBs over the range from −40 °C to 80 °C. The error bars show the standard deviations for the results from three samples. d, Voltage (red) and temperature (blue) records of the FLB when immersed in ice water and heated to the boiling point.
Extended Data Fig. 9 Electrochemical performances of the FLB textile.
a, Charge–discharge profiles of the FLB textile at discharge rates of 0.08C, 0.2C and 0.5C. b, Bending durability of FLB textiles. The specific capacities and midpoint voltages remained stable after bending, with an average capacity retention of more than 93% after bending for 100,000 cycles. The error bars show the standard deviations for the results from three samples. c, Cycling performance of the FLB textile. Both high capacities and high Coulombic efficiencies were maintained after charging and discharging for 1,000 cycles. d–f, Voltage-time curves measured for the FLB textile at 22 °C and 51% relative humidity (RH), at 80 °C and in a vacuum of −0.08 MPa, respectively.
Extended Data Fig. 10 National standard safety tests of the FLB textile.
a, The FLB textile discharged to a low voltage of 0.15 V at 2,000 mA and charged to 4.4 V. b, After reaching the fully charged state at 4.4 V, the FLB textile continued to charge to a high voltage of 6 V at 1,000 mA and was kept at 6 V for 1 h. c, The FLB textile discharged at a high current of 4,500 mA. d, The FLB textile charged at a high current of 1,500 mA after discharged to 3 V. The FLB textile did not leak, burn or explode during the safety tests.
Supplementary information
Supplementary Information
Supplementary Methods, Supplementary Figs. 1–20 and Supplementary Tables 1–3.
Supplementary Video 1
FLB textile normally charges a cellphone when cut.
Supplementary Video 2
Thirty-metre-long FLB textile.
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Lu, C., Jiang, H., Cheng, X. et al. High-performance fibre battery with polymer gel electrolyte. Nature 629, 86–91 (2024). https://doi.org/10.1038/s41586-024-07343-x
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DOI: https://doi.org/10.1038/s41586-024-07343-x
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