Ensemble Design of Electrode-Electrolyte Interfaces: Toward High-Performance Thin-Film All-Solid-State Li-Metal Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 33629830.
- Also identified by DOI 10.1021/acsnano.0c08691.
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Abstract
In accordance with the fourth industrial revolution (4IR), thin-film all-solid-state batteries (TF-ASSBs) are being revived as the most promising energy source to power small electronic devices. However, current TF-ASSBs still suffer from the perpetual necessity of high-performance battery components. While every component, a series of a TF solid electrolyte (<i>i.e</i>., lithium phosphorus oxynitride (LiPON)) and electrodes (cathode and Li metal anode), has been considered vital, the lack of understanding of and ability to ameliorate the cathode (or anode)-electrolyte interface (CEI) (or AEI) has impeded the development of TF-ASSBs. In this work, we suggest an ensemble design of TF-ASSBs using LiPON (500 nm), an amorphous TF-V<sub>2</sub>O<sub>5-<i>x</i></sub> cathode with oxygen vacancies (O<sub>vacancy</sub>), a thin evaporated Li anode (evp-Li) with a thickness of 1 μm, and an artificial ultrathin Al<sub>2</sub>O<sub>3</sub> layer between evp-Li and LiPON. Well-defined O<sub>vacancy</sub> sites, such as O(II)<sub>vacancy</sub> and O(III)<sub>vacancy</sub>, in amorphous TF-V<sub>2</sub>O<sub>5-<i>x</i></sub> not only allow isotropic Li<sup>+</sup> diffusion at the CEI but also enhance both the ionic and electronic conductivities. For the AEI, we employed protective Al<sub>2</sub>O<sub>3</sub>, which was specially sputtered using the facing target sputtering (FTS) method to form a homogeneous layer without damage from plasma. In regard to the contact with evp-Li, interfacial stability, electrochemical impedance, and battery performance, the nanometric Al<sub>2</sub>O<sub>3</sub> layers (1 nm) were optimized at different temperatures (40, 60, and 80 °C). The TF-ASSB cell containing Al<sub>2</sub>O<sub>3</sub> (1 nm) delivers a high specific capacity of 474.01 mAh cm<sup>-3</sup> under 60 °C at 2 C for the 400th cycle, and it achieves a long lifespan as well as ultrafast rate capability levels, even at 100 C; these results were comparable to those of TF Li-ion battery cells using a liquid electrolyte. We demonstrated the reaction mechanism at the AEI utilizing time-of-flight secondary ion mass spectrometry (TOF-SIMS) and molecular dynamics (MD) simulations for a better understanding. Our design provides a signpost for future research on the rational structure of TF-LIBs.