Lithiation of SiO2 in Li-Ion Batteries: In Situ Transmission Electron Microscopy Experiments and Theoretical Studies

Surface passivation has become a routine strategy of design to mitigate the chemomechanical degradation of high-capacity electrodes by regulating the electrochemical process of lithiation and managing the associated deformation dynamics. Oxides are the prevalent materials used for surface coating. Lithiation of SiO2 leads to drastic changes in its electro-chemo-mechanical properties from an electronic insulator and a brittle material in its pure form to a conductor and a material sustainable of large deformation in the lithiated form. We synthesized SiO2-coated SiC nanowires that allow us to focus on the lithiation behavior of the sub-10 nm SiO2 thin coating. We systematically investigate the structural evolution, the electronic conduction and ionic transport properties, and the deformation pattern of lithiated SiO2 through coordinated in situ transmission electron microcopy experiments, first-principles computation, and continuum theories. We observe the stress-mediated reaction that induces inhomogeneous growth of SiO2. The results provide fundamental perspectives on the chemomechanical behaviors of oxides used in the surface coating of Li-ion technologies.