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Fast charging of energy-dense lithium-ion batteries

Abstract

Lithium-ion batteries with nickel-rich layered oxide cathodes and graphite anodes have reached specific energies of 250–300 Wh kg−1 (refs. 1,2), and it is now possible to build a 90 kWh electric vehicle (EV) pack with a 300-mile cruise range. Unfortunately, using such massive batteries to alleviate range anxiety is ineffective for mainstream EV adoption owing to the limited raw resource supply and prohibitively high cost. Ten-minute fast charging enables downsizing of EV batteries for both affordability and sustainability, without causing range anxiety. However, fast charging of energy-dense batteries (more than 250 Wh kg1 or higher than 4 mAh cm2) remains a great challenge3,4. Here we combine a material-agnostic approach based on asymmetric temperature modulation with a thermally stable dual-salt electrolyte to achieve charging of a 265 Wh kg1 battery to 75% (or 70%) state of charge in 12 (or 11) minutes for more than 900 (or 2,000) cycles. This is equivalent to a half million mile range in which every charge is a fast charge. Further, we build a digital twin of such a battery pack to assess its cooling and safety and demonstrate that thermally modulated 4C charging only requires air convection. This offers a compact and intrinsically safe route to cell-to-pack development. The rapid thermal modulation method to yield highly active electrochemical interfaces only during fast charging has important potential to realize both stability and fast charging of next-generation materials, including anodes like silicon and lithium metal.

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Fig. 1: Figure of merit of fast charging batteries.
Fig. 2: ATM cycles of energy-dense LiBs.
Fig. 3: Fast charging of energy-dense LiBs with enhanced ion transport.
Fig. 4: Electrochemical–thermal coupled simulations of a 12S1P pack of 150 Ah prismatic cells.

Data availability

All data generated or analysed during this study are included in this published article, the Extended Data and the Supplementary Information.

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Acknowledgements

Partial support from the US Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under award no. DE-EE0008355, the William E. Diefenderfer Endowment and Air Force STTR under contract FA864921P1620 is gratefully acknowledged. We are also grateful to Gamma Technologies for offering GT-AutoLion software.

Author information

Authors and Affiliations

Authors

Contributions

C.Y.W., T.L., B.D.M. and E.S.R. wrote the manuscript. S.G. designed and built the cells. T.L. and X.G.Y. designed the experiments. T.L. built the test stand and carried out the experiments. Y.L. optimized electrolytes in coin cells. C.Y.W., N.V.S. and B.D.M. designed and performed 3D numerical simulations. All authors contributed to development of the manuscript and to discussions as the project developed.

Corresponding authors

Correspondence to Chao-Yang Wang or Brian D. McCarthy.

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Competing interests

B.D.M., E.S.R., N.V.S. and C.Y.W. have a financial interest in EC Power.

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Extended data figures and tables

Extended Data Fig. 1 LiB design for ATM cycling.

a, LiB with an embedded nickel foil for internal heating. Before each charging, current goes through the internal heating structure and heats up the cell to 65 °C in less than one minute. After reaching the target temperature, the charging channel starts to take in energy and maintains thermal balance throughout the charging process. b, Cell and heating-foil temperatures versus heating time. A heating rate of 0.75 °C s−1 was achieved when applying 3.3 V on the heating channel.

Extended Data Fig. 2 Rate performance tests and model validation.

a, Cell with baseline electrolyte. b, Cell with dual-salt electrolyte; the simulated transference number was 0.48.

Extended Data Fig. 3 Ageing mechanisms under ATM cycling.

a, b, Lithium plating detection with voltage relaxation method for 4.2 mAh cm2 LiBs and 3.4 mAh cm−2 LiBs. c, d, Coulombic efficiency during cycling. e, f, Change of resistance attained by EIS tests. Baseline electrolyte was used in these tests.

Extended Data Fig. 4 Numerical prediction of lithium plating at various charge rates with T=60°C.

a, Experimental and simulated voltage profiles for baseline cells. b, Simulated lithium deposition potential for baseline cells. c, Experimental and simulated voltage profiles for cells with dual-salt electrolyte. d, Simulated lithium deposition potential for cells with dual-salt electrolyte.

Extended Data Fig. 5 Ageing mechanisms under fast charging of batteries with enhanced ion transport.

a, Lithium plating detection with voltage relaxation method for 3.4 mAh cm−2 LiBs with enhanced ion transport. b, Coulombic efficiency during cycling. c, Change of resistance attained by EIS tests.

Extended Data Fig. 6 Fast charging cycling with different combinations of electrodes and electrolytes.

Use of either the mixed dual-salt electrolyte or higher porosity anodes failed to give long cycle lifetime; both were required for long cycle lifetime.

Extended Data Fig. 7 Parameter map of lithium plating-free (LPF) charging (3.4 mAh cm2).

a, Simulated LPF region given by relative ion transport resistance and charge transfer resistance when 3C charging the battery (*denotes unitless variables, referenced with the properties of a fresh baseline cell charging at 60 °C). b, Simulated LPF region given by relative ion transport resistance and charge transfer resistance when 4C charging the battery, in which the open symbol labelled as 65 °C denotes the high porosity anode. c, Change of charge transfer resistance during aging attained from EIS tests and analysis. d, Change of ion transport resistance during ageing attained from EIS tests and analysis.

Extended Data Fig. 8 Effects of heat transfer coefficient.

Effects during C/3 discharge on 4C charge - C/3 discharge cycling under otherwise the cooling condition of 140 W per m2K, indicative of dramatic shortening in time for the battery to cool down to below 40 °C. Note that a heat transfer coefficient of 300 W per m2K is still attainable by strong aspirated air convection. a, Cell temperature curves. b, Cell voltage curves. c, Spatial temperature nonuniformity, TmaxTmin, as a function of time.

Extended Data Fig. 9 EIS tests and equivalent circuit for fitting.

a, Typical shape and interpretation for cell impedance in the complex plane. b, Equivalent circuit and the mathematical expression to fit the experimental results. c, EIS results and fitting curve for baseline cell under ATM cycling with 3C charging to 80% SOC. d, EIS results and fitting curve for cell with enhanced ion-transport under ATM cycling with 4C charging to 70% SOC. e, EIS results and fitting curve for cell with enhanced ion-transport under ATM cycling with 4C charging to 75% SOC.

Supplementary information

Supplementary Information

Cell design details, Tables 1–4, Figures 1–5, the electrochemical–thermal coupled model and equivalent circuit for EIS.

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Wang, CY., Liu, T., Yang, XG. et al. Fast charging of energy-dense lithium-ion batteries. Nature 611, 485–490 (2022). https://doi.org/10.1038/s41586-022-05281-0

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