High-energy density Li-ion batteries (LIBs) are expected to respond to the increasing energy demand related to the fast-growing industry of portable electronic devices, electric vehicles, and smart grid applications, as well as wearable devices and medical implants. The use of high-voltage cathodes, working up to 5 V and beyond, is probably the most straightforward way to achieve this purpose. Being the spinel LiNi 0.5 Mn 1.5 O 4 (LNMO), with a theoretical specific capacity of 147 mAh g −1 , the top choice for the next generation of highenergy density LIBs. [1] However, the main strength of this material, namely, its high operating voltage ≈4.7 V nested in the redox potential of the Ni 2+/3+ and Ni 3+/4+ couples, [2] is also the origin of its main limitation: the decomposition at high voltages of the liquid electrolytes used in standard LIBs. In this sense, solid state batteries represent a valid solution stemmed, among others, on the wide electrochemical stability window displayed by some solid electrolytes. [3,4] Within this category, the case of thin-film solid state batteries [5,6] is of great interest, especially for certain thin-film electrolytes that would present manufacturing advantages at industrial level, [7][8][9] thus enabling the production and commercialization of the next generation Li-ion batteries. The fabrication method and the battery configuration will also be important factors to consider. A paradigm shift in terms of electrode fabrication methods and battery architecture is needed if new horizons are going to be reached, for example, concerning solvent-and additive-free electrodes, faster production methods, and/or more efficient use of the raw materials in the battery fabrication process.Atomic layer deposition (ALD) is considered the premier technique for processing thin-film components owing to its surface conformality, repeatability, scalability, and delivery of pinhole-free coatings. [10] Indeed, its suitability has been demonstrated for the fabrication of several solid electrolytes, including
The substitution of an organic liquid electrolyte with lithium-conducting solid materials is a promising approach to overcome the limitations associated with conventional lithium-ion batteries. These constraints include a reduced electrochemical stability window, high toxicity, flammability, and the formation of lithium dendrites. In this way, all-solid-state batteries present themselves as ideal candidates for improving energy density, environmental friendliness, and safety. In particular, all-solid-state configurations allow the introduction of compact, lightweight, high-energy-density batteries, suitable for low-power applications, known as thin-film batteries. Moreover, solid electrolytes typically offer wide electrochemical stability windows, enabling the integration of high-voltage cathodes and permitting the fabrication of higher-energy-density batteries. A high-voltage, all-solid-state lithium-ion thin-film battery composed of LiNi 0.5 Mn 1.5 O 4 cathode, a LiPON solid electrolyte, and a lithium metal anode has been deposited layer by layer on low-cost stainless-steel current collector substrates. The structural and electrochemical properties of each electroactive component of the battery had been analyzed separately prior to the full cell implementation. In addition to a study of the internal solid−solid interface, comparing them was done with two similar cells assembled using conventional lithium foil, one with thin-film solid electrolyte and another one with thin-film solid electrolyte plus a droplet of LP30 liquid electrolyte. The thin-film all-solid state cell developed in this work delivered 80.5 mAh g −1 in the first cycle at C/20 and after a C-rate test of 25 cycles at C/10, C/5, C/2, and 1C and stabilized its capacity at around 70 mAh g −1 for another 12 cycles prior to the start of its degradation. This cell reached gravimetric and volumetric energy densities of 333 Wh kg −1 and 1,212 Wh l −1 , respectively. Overall, this cell showed a better performance than its counterparts assembled with Li foil, highlighting the importance of the battery interface control.
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