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Atomic layer deposition for lithium-ion batteries
Abstract
In this work, thin films have been deposited using atomic layer deposition for energy applications, more specifically, for lithium-ion battery applications, and the goal of this work is to illustrate the strengths and weaknesses, the highlights and pitfalls, and the advantages and drawbacks of using ALD in lithium-ion battery development.
... In order to build a battery on a complex 3D structure, a deposition technique is required that can achieve excellent conformality. Atomic layer deposition is such a technique and is being widely investigated in this context [46][47][48]. ...
... Proper surface engineering is capable of stabilizing these interfaces and improving the cycle life and rate performance of the electrodes [49]. ALD coatings are extensively studied in this context [48,50]. A nice example is how a few ALD alumina cycles can improve the capacity retention of a lithium cobalt oxide electrode (figure 1.11) [51]. ...
... 6 These qualities make ALD an ideal technique to deposit electrode materials for LIBs. 7 The stoichiometric cubic spinel LiMn 2 O 4 crystallizes in a space group Fd3m (Figure 1). The oxygen anions arrange in a cubic closed-packed structure, leaving two possible interstitial sites for the metal cations (denoted by Wyckoff symbols 8 ): tetrahedral 8a, which are occupied by lithium ions, and octahedral 16d, which are filled with manganese cations. ...
LiMn2O4 is a promising candidate for a cathode material in lithium ion batteries (LIBs) due to its ability to intercalate lithium ions reversibly through its three-dimensional manganese oxide network. One of the promising techniques for depositing LiMn2O4 thin film cathodes is atomic layer deposition (ALD). Due to its unparalleled film thickness control and film conformality, ALD helps to fulfill the industry demands for smaller devices, nanostructured electrodes and all-solid-state batteries. In this work the intercalation mechanism of Li⁺ ions into an ALD grown β-MnO2 thin film was studied. Samples were prepared by pulsing LiOtBu and H2O for different cycle numbers onto about 100 nm thick MnO2 films at 225 ºC and characterized with X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), X-ray reflectivity (XRR), time-of-flight elastic recoil detection analysis (TOF-ERDA) and residual stress measurements. It is proposed that for < 100 cycles of LiOtBu/H2O the Li⁺ ions penetrate only to the surface region of the β-MnO2 film and the samples form a mixture of β-MnO2 and a lithium deficient non-stoichiometric spinel phase LixMn2O4 (0 < x < 0.5). When the lithium concentration exceeds x ≈ 0.5 in LixMn2O4 (corresponding to 100 cycles of LiOtBu/H2O), the crystalline phase of manganese oxide changes from the tetragonal pyrolusite to the cubic spinel, which enables Li⁺ ions to migrate throughout the whole film. Annealing in N2 at 600 ºC after the lithium incorporation seemed to convert the films completely to the pure cubic spinel LiMn2O4.
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