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Unlocking Stable Multi-Electron Cycling in NMC811 Thin-Films between 1.5 – 4.7 V

机译:Unlocking Stable Multi-Electron Cycling in NMC811 Thin-Films between 1.5 – 4.7 V

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摘要

Among cathode materials, LiNi_(0.8)Mn_(0.1)Co_(0.1)O_2 (NMC811) is the most discussedfor high performance Li-ion batteries, thanks to its capacity of ≈200 mAh g~(-1)and low Co content. Here, it is demonstrated that NMC811 can reversiblyaccommodate more than one Li-ion per formula unit when coupled with asolid-state electrolyte, thus significantly increasing its capacity. Sputtered Li-richNMC811 cathodes are tested with lithium–phosphorus–oxynitride as a solidstateelectrolyte in a thin-film architecture, which is a simplified 2D model withdirect access to the cathode-electrolyte interface. The solid-state electrolytehelps to stabilize the interface and prevents capacity fading, voltage decay, andinterface resistance growth, thus allowing cycling at extended voltage ranges of1.5–4.7 V. While the liquid electrolyte cells suffer from rapid capacity decay, theLi-rich NMC811 cells with the solid-state electrolyte can cycle at a fast rate andan initial capacity of 149 mAh g-1 from 1.5 to 4.3 V for 1000 cycles. The all-solidstatethin-film cells with a lithium metal anode yield a discharge capacity ofup to 350 mAh g~(-1) at C/10 because of multi-electron cycling with a coulombicefficiency of 90.1%. The results demonstrate how solid-state electrolytes thatare stable against NMC811 cathodes can unlock the full potential of this Li-richand Ni-rich cathode class.

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