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Real-Time Stress Measurement in SiO2 Thin Films during Electrochemical Lithiation/Delithiation Cycling

Siva P V Nadimpalli's picture

Real-Time Stress Measurement in SiO2 Thin Films during Electrochemical Lithiation/Delithiation Cycling


    S. Rakshit, R. Tripuraneni, Siva P. V. Nadimpalli

Abstract: Oxide coatings have been shown to improve the cyclic performance of high-energy density electrode materials such as Si. However, no study exists on the mechanical characterization of these oxide coatings. Here, thin film SiO2 electrodes are cycled under galvanostatic conditions (at C/9 rate) in a half-cell configuration with lithium metal foil as counter/reference electrode, with 1 M LiPF6 in ethylene carbonate, diethyl carbonate, dimethyl carbonate solution (1:1:1, wt%) as electrolyte. Stress evolution in the SiO2 thin film electrodes during electrochemical lithiation/delithiation is measured in situ by monitoring the substrate curvature using a multi-beam optical sensing method. Upon lithiation SiO2 undergoes extensive inelastic deformation, with a peak compressive stress of 3.1 GPa, and upon delithiation the stress became tensile with a peak stress of 0.7 GPa. A simple plane strain finite element model of Si nanotube coated with SiO2 shell was developed to understand the mechanical response of the core-shell type microstructures under electrochemical cycling; measured stress response was used in the model to represent SiO2 constitutive behavior while Si was treated as an elastic-plastic material with concentration dependent mechanical properties obtained from the literature. The results reported here provide insights and quantitative understanding as to why the highly brittle SiO2coatings are able to sustain significant volume expansion (300%) of Si core without fracture and enhance cyclic performance of Si reported in the literature. Also, the basic mechanical properties presented here are necessary first step for future design and development of durable Si/SiO2 core shell structures or SiO2-based electrodes.

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