A critical current density on stripping is identified that results in dendrite formation on plating and cell failure. When the stripping current density removes Li from the interface faster than it can be replenished, voids form in the Li at the interface and accumulate on cycling, increasing the local current density at the interface and ultimately leading to dendrite formation on plating, short circuit and cell death. This occurs even when the overall current density is considerably below the threshold for dendrite formation on plating. For the Li/Li6PS5Cl/Li cell, this is 0.2 and 1.0 mA cm−2 at 3 and 7 MPa pressure, respectively, compared with a critical current for plating of 2.0 mA cm−2 at both 3 and 7 MPa. The pressure dependence on stripping indicates that creep rather than Li diffusion is the dominant mechanism transporting Li to the interface. The critical stripping current is a major factor limiting the power density of Li anode solid-state cells. Considerable pressure may be required to achieve even modest power densities in solid-state cells.
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Supporting research data has been deposited in the Oxford Research Archive and is available at https://doi.org/10.5287/bodleian:gA47ppAz9.
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P.G.B. is indebted to the Faraday Institution All-Solid-State Batteries with Li and Na Anodes (FIRG007, FIRG008), as well as the Engineering and Physical Sciences Research Council (EPSRC), including the SUPERGEN Energy Storage Hub (EP/L019469/1), Enabling Next Generation Lithium Batteries (EP/M009521/1), the University of Oxford experimental equipment upgrade (EP/M02833X/1) and the Henry Royce Institute for capital equipment (EP/R010145/1) for financial support. The authors thank Dr Phil Holdway, Oxford Materials Characterisation Service, for help with XPS measurements.
The authors declare no competing interests.
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Kasemchainan, J., Zekoll, S., Spencer Jolly, D. et al. Critical stripping current leads to dendrite formation on plating in lithium anode solid electrolyte cells. Nat. Mater. 18, 1105–1111 (2019). https://doi.org/10.1038/s41563-019-0438-9
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