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Scalable production of high-performing woven lithium-ion fibre batteries

Abstract

Fibre lithium-ion batteries are attractive as flexible power solutions because they can be woven into textiles, offering a convenient way to power future wearable electronics1,2,3,4. However, they are difficult to produce in lengths of more than a few centimetres, and longer fibres were thought to have higher internal resistances3,5 that compromised electrochemical performance6,7. Here we show that the internal resistance of such fibres has a hyperbolic cotangent function relationship with fibre length, where it first decreases before levelling off as length increases. Systematic studies confirm that this unexpected result is true for different fibre batteries. We are able to produce metres of high-performing fibre lithium-ion batteries through an optimized scalable industrial process. Our mass-produced fibre batteries have an energy density of 85.69 watt hour per kilogram (typical values8 are less than 1 watt hour per kilogram), based on the total weight of a lithium cobalt oxide/graphite full battery, including packaging. Its capacity retention reaches 90.5% after 500 charge–discharge cycles and 93% at 1C rate (compared with 0.1C rate capacity), which is comparable to commercial batteries such as pouch cells. Over 80 per cent capacity can be maintained after bending the fibre for 100,000 cycles. We show that fibre lithium-ion batteries woven into safe and washable textiles by industrial rapier loom can wirelessly charge a cell phone or power a health management jacket integrated with fibre sensors and a textile display.

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Fig. 1: Measured and predicted internal resistances of FLIBs decrease with fibre length.
Fig. 2: Continuous fabrication and structural characterization of long FLIBs.
Fig. 3: Electrochemical properties of FLIBs.
Fig. 4: Applications of FLIB textiles.

Data availability

The data that support the findings of this study are available from figshare at https://figshare.com/articles/online_resource/Source_data_FLIBs/14775900Source data are provided with this paper.

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Acknowledgements

This work was supported by Ministry of Science and Technology of the People’s Republic of China (2016YFA0203302), National Natural Science Foundation of China (21634003, 22075050, 21805044), Science and Technology Commission of Shanghai Municipality (20JC1414902, 18QA1400700, 19QA1400800) and Shanghai Municipal Education Commission (2017-01-07-00-07-E00062). We thank Ai Lin Chun of Science Storylab for critically reading and editing the manuscript.

Author information

Affiliations

Authors

Contributions

H.P. directed all aspects of the project. H.P. and P.C. conceived and designed the project. J.H. and C.L. performed the experiments on fabrication of FLIBs and integration systems. X.S. and J. Wu performed the fabrication of display textile. F.H., L.W., J. Wang and H.Y. performed the fabrication of fibre sensors. J.H., C.L. and H.J. analysed the data. Y.Z., T.C., G.Z., X.S., B.W., Y.W., Y.X. and all other authors discussed the data. J.H., C.L., P.C. and H.P. wrote the paper.

Corresponding authors

Correspondence to Peining Chen or Huisheng Peng.

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Competing interests

The authors declare no competing interests.

Additional information

Peer review information Nature thanks Kun Fu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Extended data figures and tables

Extended Data Fig. 1 Preliminary FLIBs.

a, Schematic illustration of FLIB with a twisted structure. The typical active materials of LCO and graphite were coated on the aluminium and copper wires to form positive and negative fibre electrodes, respectively. The negative fibre electrode was wrapped with commercial separator film to prevent short circuit. b, Photograph of a FLIB. Scale bar, 4 mm. c, Disassembled FLIB to show the components such as positive electrode, negative electrode, separator and encapsulation tube. Scale bar, 4 mm. d, Photograph of FLIBs with different lengths. e, Relationship between the internal resistance of FLIB and the battery length. Error bars: standard deviations of the results from three samples

Source data.

Extended Data Fig. 2 Length dependence of internal resistance of FLIB under different conditions.

a–c, Length dependence of internal resistance for FLIBs using LCO/graphite (a), LiNi0.5Co0.2Mn0.3O2 (NCM523)/graphite (b), and LCO/SiO-graphite composites (SiC650) (c) as electrode materials. d–f, Length dependence of internal resistance of empty charged state (d), half charged state (e), and fully charged state (f) for LCO/graphite. g–i, Length dependence of internal resistance with increasing lithium salt concentrations of 0.01 M (g), 0.1 M (h) and 1 M (i) in electrolyte for LCO/graphite. Error bars: standard deviations of the results from three samples

Source data.

Extended Data Fig. 3 Internal resistance of FLIB measured by EIS method.

a, Typical Nyquist plots of FLIBs with different lengths. The FLIBs show the same lithium-ion concentration of 1 M in electrolyte and charged state of 50%. b, Z values along the fibre length of an LCO/graphite FLIB. Here, L is the investigated length on a FLIB with a length of L0. Z was obtained by measuring the polarization resistance of FLIB through EIS analysis, that is, it was calculated as a sum of interface resistance and charge transfer resistance from the equivalent circuit simulation curve of the Nyquist plot. Error bars: standard deviations of the results from three samples. c, Internal resistances of FLIBs obtained from EIS correlate linearly (y = 1.06047x; R2 = 0.99663) with predicted values. Error bars: standard deviations of the results from three samples. d–f, Internal resistance of LCO/graphite (d), NCM523/graphite (e) and LCO/SiC650 (f) FLIBs as a function of length. g–i, Internal resistance of LCO/graphite FLIB at empty charged state (g), half charged state (h) and fully charged state (i). j–l, Internal resistance of LCO/graphite FLIB with increasing lithium salt concentrations of 0.01 M (j), 0.1 M (k) and 1 M (l) in electrolyte. Error bars: standard deviations of the results from three samples

Source data.

Extended Data Fig. 4 Continuous coating of fibre electrodes.

a, Binder ratio dependence of deformation parameter for the beads on the fibre electrode. With increasing binder contents, the beads disappeared, and the electrode surface turned smooth. Deformation parameter D = (L − B)/(L+B), where L is bead size along the fibre and B is bead size in the radial direction of the fibre. Scale bar, 500 μm. b, Photographs of fluid coating process. (i) Photograph of fibre fluid coating machine. Scale bar, 30 cm. (ii–iv) Photographs of detailed coating processes. Scale bar, 5 cm. c, d, SEM images show that bending of positive (c) and negative (d) fibre electrodes with a curvature radius of 1.5 mm did not cause any peeling or cracks in the active layer. Scale bars, from left to right, 2 mm (i), 500 μm (ii) and 100 μm (iii). e, f, SEM images of positive and negative fibre electrode after bending for 100,000 cycles with a curvature radius of 1 cm. Scale bar, 500 μm. g, LCO loading weight and corresponding discharge capacity retention (1 C rate) for five different electrodes. Capacity retention remained stable at first and then decreased with increasing LCO loading weight. Error bars: standard deviations of the results from three samples. h, i, Charge–discharge profiles of LCO/Li (h) and graphite/Li (i) of coin cells

Source data.

Extended Data Fig. 5 Assembly of fibre electrodes.

a–c, Separator wrapping angle of 27° (a), 22° (b) and 16° (c). Scale bars, 10 cm. d–f, SEM images of wrapped negative fibres with wrapping angles of 27° (d), 22° (e) and 16° (f). Scale bars, 500 μm. When the wrapping angle was 16°, the negative fibre electrode was fully covered by the separator strip without excessive overlap. g–j, Photographs of twisted fibre electrodes with pitches of 4 mm (g), 3 mm (h), 2 mm (i) and 1.5 mm (j). Scale bar, 4 mm. k–n, SEM images of twisted fibre electrodes with pitches of 4 mm (k), 3 mm (l), 2 mm (m) and 1.5 mm (n). o, Internal resistances of 20-cm-long FLIBs with different twisting pitches. Error bars represent the standard deviations of the results from three samples. p, Capacity retention of FLIBs with pitches from 4 mm to 1.5 mm at different applied discharge rate. FLIBs with a large pitch cause high internal resistance, but too small a pitch would result in peeling of active materials. q, Photograph of twisted fibre electrodes with a pitch of 2 mm. Scale bar, 2 mm. ru, Statistical distributions for twisted fibre electrodes with different pitches of 4 mm (r), 3 mm (s), 2 mm (t) and 1.5 mm (u)

Source data.

Extended Data Fig. 6 Encapsulation of FLIB.

a, Illustration of extruder. The right top and bottom photographs show twisted fibre electrodes being inserted into extrusion die and encapsulating electrodes through extruding polymer composite tube. Scale bar, 2 cm. b, Cross-sectional SEM image of fibre electrodes with encapsulation tube, which had an outer diameter of 1.5 mm with tube thickness of 0.25 mm. Scale bar, 500 μm. c, Schematic showing the injection pump and the tip-forming machine. d, Schematic showing the set-up of the tip-forming machine used to encapsulate the end of the FLIBs. One end of the FLIB is inserted into the sealing hole (i, ii) and heated at 300 °C for 5 s (iii). Upon cooling, a smooth and solid end is formed (iv). e, Photograph of the end of an encapsulated tube. Electrolyte is in red. Scale bar, 1 cm. f, No obvious electrolyte leakage from the end of the encapsulated tube was observed when submerged in water. Scale bar, 1 cm. g, Tensile strength of the encapsulation tube remained largely unchanged after being immersed in the electrolyte for different durations. σ0 and σ represent tensile strengths before and after immersion, respectively. Error bars are standard deviations of the results from five samples. h, Photograph of the standard washing machine and washing container for the washing test. Scale bars, from left to right, 20 cm and 5 cm. i, Photograph of drying equipment. Scale bar, 30 cm. j, Tensile strength of the encapsulation tube remained unchanged after several washing and drying cycles. σ0 and σ represent the tensile strengths before and after washing, respectively. Error bars are standard deviations of the results from five samples

Source data.

Extended Data Fig. 7 Test report of FLIB.

a, b, Scanned copies of the independent confirmation report (a) and appendix (b) showing the capacity and energy density of FLIB. Discharge capacity is required by the testing standard authorized by China National Accreditation Service for Conformity Assessment (CNAS) and China Inspection Body and Laboratory Mandatory Approval (CMA), while discharge energy is not required. The remark “The discharge energy test is beyond the independent confirmation range of CNAS and CMA” in the independent confirmation report simply indicates that discharge energy test is not a requirement within the testing standard.

Extended Data Fig. 8 Electrochemical stability and durability of FLIBs.

a, Capacity retention of FLIBs from −20 °C to 60 °C. Error bars represent the standard deviations of the results from three samples. b, Stress–strain curve shows an LCO/graphite FLIB has a tensile strength of around 89 MPa and elongation of around 13%. c, Photographs of a FLIB being dynamically bent at a frequency of 2.5 Hz while its open-circuit voltage was traced during the bending cycle. d, e, Charge and discharge profiles of the FLIB under dynamic bending (at 2.5 Hz) are stable with no obvious fluctuations. f, Capacity retention of gel-electrolyte-based FLIB reaching >90% after 100,000 bending cycles. Error bars: standard deviations of the results from three samples. Insets: charge–discharge profiles at the 1st, 100th and 100,000th bending cycle

Source data.

Extended Data Fig. 9 Fabrication of FLIB textile, and FLIB textile charging a tablet computer under harsh conditions.

a–d, Textile made from FLIBs by a commercial rapier loom. a, b, Fabrication process using a rapier loom (inset, rolling-up of a textile). Scale bar, 10 cm. c, Photograph of a 5-m-long, 0.3-m-wide FLIB textile. d, Photograph of FLIB textile with different styles. Scale bar, 2 cm. e, FLIB textile charging a tablet as normal, even when folded. i, FLIB textile charging tablet; ii, charging tablet after two folds; iii, charging tablet after three folds. The size of the textile was 0.3 m long × 0.5 m wide. f, FLIB textile charging tablet under car crushing. The car mass was about 1,300 kg. g, FLIB textile being washed by a washing machine. Scale bar, 10 cm. h, FLIB textile charging a tablet after washed and dried. i, FLIB textile charging tablet when punctured by a blade. j, k, The temperature of the zone monitored by the infrared imager remains almost unchanged before (j) and after puncture (k). l, Photograph of FLIB textile wirelessly charging a cell phone at 40 °C. FLIB textile was heated with a hot stage. m, Infrared thermal images of FLIB textile during wireless charging of cell phone.

Extended Data Fig. 10 Fabrication of a health management system integrated with fibre sweat sensors and an electroluminescent textile display.

a, b, Sweat fibre sensors integrated with Na+, Ca2+ working fibre electrodes and Ag/AgCl reference fibre electrode. Scale bar, 1 cm. c, d, Calibration plot for Na+ (c) and Ca2+ (d). The ion concentration was converted from the potential signal according to the calibration plot. e, f, Photographs of the sewing machine (e) and electroluminescent yarn (f) used to fabricate electroluminescent textile display. Scale bar, 5 cm

Source data.

Extended Data Table 1 Key performances of FLIB and typical commercial batteries

Supplementary information

Supplementary Information

This file contains Supplementary Figures 1 – 3 and Supplementary Tables 1 – 6.

Supplementary Video 1

Production process of FLIBs.

Supplementary Video 2

FLIB textile wirelessly charges a smart phone.

Supplementary Video 3

FLIB textile stably charges a pad under folding.

Supplementary Video 4

FLIB textile normally charges a pad after washing.

Supplementary Video 5

FLIB textile normally charges a pad when punctured by blade.

Supplementary Video 6

A jacket woven with FLIBs wirelessly charges a smart phone.

Source data

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He, J., Lu, C., Jiang, H. et al. Scalable production of high-performing woven lithium-ion fibre batteries. Nature 597, 57–63 (2021). https://doi.org/10.1038/s41586-021-03772-0

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