Optimal Microstructure of Silicon Monoxide as the Anode for Lithium-Ion Batteries

Because of its metastable nature, silicon monoxide (SiO) consists of Si nanodomains in an amorphous matrix of SiO2. The microstructure of SiO, including SiO2, Si domains, and interphase (SiOx) between domains, was modified via an annealing treatment in argon gas and thoroughly characterized by in-situ and ex-situ X-ray diffraction, pair distribution function, and electron energy loss spectroscopy. Two microstructure transformation routes were observed during the annealing process: (1) at a temperature of <800 °C, the annealing treatment was found to affect mainly the structural conformation of the amorphous SiO2 matrix and the interphase, while (2) an annealing temperature of >800 °C led to significant Si nanodomain growth. We found that the microstructure has a great impact on the electrochemical performance of SiO. The optimized microstructure of SiO appears to be achieved through annealing treatment at 800 °C or less, which results in interphase (SiOx) reduction without causing significant Si domain growth. This work provides a deep insight into the domain and interphase transformation of SiO upon heat treatment. The improved understanding of the relationship between SiO microstructure and its electrochemical behavior will enable proper design and development of high-energy SiO for lithium-ion batteries.