Review on Computational-Assisted to Experimental Synthesis, Interfacial Perspectives of Garnet-Solid Electrolytes for All-Solid-State Lithium Batteries

The future state-of-art for energy storage materials is essentially credited to the development of inorganic electrochemical stable solid-state electrolytes (SSEs). All-solid-state lithium batteries (ASSLBs) have been anticipated to be mainly promising a new generation battery technology, owing to the wide range of voltage window, superior safety, and long cyclic performance. Lithium-containing oxide-based garnet (Li7La3Zr2O12) material has become a fascinating potential candidate for ASSLBs as SSEs due to their high ionic conductivity and stability against lithium anode and high capacity cathodes. This review focuses on the computational-guided evolution approaches and screening high-performance garnet materials, showcases all conventional to modern experimental methods, structural studies, and strategies to improve the ionic conductivity of the newly designed garnet SSEs. The panoramic view of chemical instability and developments in interfacial engineering between the cathode/anode and solid-state garnet electrolytes treated via different methods are systematically discussed. The main gaps between lab-scale to large-scale batteries in the integral technology chains, including synthesis technique of solid electrolyte, battery designing, and assembly steps, are identified. Furthermore, we summarize the up-to-date applications of the garnet SSEs and future perspectives to explore the methodologies to develop the ideal garnet solid electrolytes and their commercial applications in ASSLBs.