reversible capacity of current cathodes is lower than that of conventional graphite anodes (372 mAh g -1 ) and far behind that of high-capacity anodes such as lithium metal (3860 mAh g -1 ) and silicon (4200 mAh g -1 ). [2,3] Simultaneously, the cathode is the main contributor to the material cost at the cell level. [4] Currently, LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) is gaining commercial adoption due to its capacity of ≈200 mAh g -1 assuming one Li-ion per formula unit and low content of expensive cobalt. [5] Two intriguing research questions stand out: i) Is it possible to increase the cathodic discharge capacity by introducing additional lithium into the host NMC811 structure? ii) Can we control the reactivity of Ni-rich cathode material with the electrolyte and prevent the formation of a solid electrolyte interphase (SEI) layer and consequent low capacity retention? [6,7] NMC cathodes can actually store more than one lithium ion per formula unit. This phenomenon is by no means a recent discovery, and the first reports of Li-rich NMC-type layered oxide cathodes date back to 2003. [8] When discussing Li-rich layered cathode materials, it is important to differentiate between Mn-based and Ni-based compositions. Most of the investigated Li-rich NMC compounds are based on Mn as main redox-active transition metal. [9,10] This allows for excess lithium to be stored in a Li 2 MnO 3 composite structure embedded in Li(Ni, Mn, Co)O 2 , where oxygen atoms are involved in the redox process above 4.5 V. [11] Such Among cathode materials, LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) is the most discussed for 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 reversibly accommodate more than one Li-ion per formula unit when coupled with a solid-state electrolyte, thus significantly increasing its capacity. Sputtered Li-rich NMC811 cathodes are tested with lithium-phosphorus-oxynitride as a solidstate electrolyte in a thin-film architecture, which is a simplified 2D model with direct access to the cathode-electrolyte interface. The solid-state electrolyte helps to stabilize the interface and prevents capacity fading, voltage decay, and interface resistance growth, thus allowing cycling at extended voltage ranges of 1.5-4.7 V. While the liquid electrolyte cells suffer from rapid capacity decay, the Li-rich NMC811 cells with the solid-state electrolyte can cycle at a fast rate and an initial capacity of 149 mAh g -1 from 1.5 to 4.3 V for 1000 cycles. The all-solidstate thin-film cells with a lithium metal anode yield a discharge capacity of up to 350 mAh g -1 at C/10 because of multi-electron cycling with a coulombic efficiency of 90.1%. The results demonstrate how solid-state electrolytes that are stable against NMC811 cathodes can unlock the full potential of this Li-rich and Ni-rich cathode class.
Lithiated Nb, Al, or Ti metal oxide interlayers improve the LiCoO2/LLZO interface, whereby the Li–Nb–O interlayer exhibits the highest performance.
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