Alloying anodes are of great interest as a replacement for graphite in lithium-ion batteries (LIBs) since they can store one or more Li atoms per host atom. Si has received the most attention in this regard due to its very high theoretical specific capacity (3579 mAh/g, ~8300 mAh/cm3)1 and relatively low cost. However, the durability of batteries with high Si content is limited due to the unstable solid-electrolyte interphase (SEI) on Si2 and its large volume change upon lithiation and delithiation which leads to cracking and pulverization3, 4. Among alloying anodes, amorphous materials generally outperform crystalline materials5, 6. The absence of grain boundaries can improve passivity7-9, and amorphous materials generally lithiate in a continuous manner, which eliminates phase boundaries and the mechanical strains associated with them. In addition, amorphous materials composed solely of metals and/or metalloid elements, termed metallic glasses, have been shown to exhibit exceptional hardness, yield strength, and fracture toughness7-9.This study explores an Al-Si-Mn glass as an alternative LIB anode. Si-based metallic glasses are appealing because they maintain Si, which can alloy with up to 3.75 Li6, 10, as the main Li-binding element, but distribute it homogeneously within an amorphous matrix. A dense amorphous Al64Si25Mn11 metallic glass (a-AlSiMn) was successfully produced via splat quenching, a rapid cooling technique that is scalable and commonly used to produce amorphous materials for a variety of applications. This process is shown schematically in the figure below. The a-AlSiMn glass exhibits greater specific capacity (>900 mAh/g) than graphite and a low lithiation potential, making it suitable for high-energy density LIBs. The glass remains amorphous throughout cycling, maintaining any improved mechanical properties conferred by the amorphous structure.Crucially, parasitic electrolyte reduction is found to be much reduced in comparison to pure Si or Al, and comparable to that on Cu. The charge consumed by electrolyte reduction in each cycle is given in the figure below for a-AlSiMn and an amorphous Si reference anode. The resulting SEI on a-AlSiMn is very thin, and rich in fluorinated species such as LiF, F-P-O groups, and fluorinated oxides of silicon and aluminum, whereas very few organic species are present. In particular, lithium ethylene decarbonate (LiEDC), which plays a large role in SEI formation on Si, is entirely absent, and a thinner, more stable SEI results. This study shows that metallic glasses can become a viable new class of alloying anode materials for LIBs with improved surface passivity. Li, J.; Dahn, J. R., An In Situ X-Ray Diffraction Study of the Reaction of Li with Crystalline Si. Journal of The Electrochemical Society 2007, 154 (3), A156.Yin, Y.; Arca, E.; Wang, L.; Yang, G.; Schnabel, M.; Cao, L.; Xiao, C.; Zhou, H.; Liu, P.; Nanda, J.; Teeter, G.; Eichhorn, B. W.; Xu, K.; Burrell, A. K.; Ban, C., Non-Passivated Silicon Anode Surface. ACS applied materials & interfaces 2020.Kasavajjula, U.; Wang, C.; Appleby, A. J., Nano- and bulk-silicon-based insertion anodes for lithium-ion secondary cells. Journal of Power Sources 2007, 163 (2), 1003-1039.Liang, B.; Liu, Y.; Xu, Y., Silicon-based materials as high capacity anodes for next generation lithium ion batteries. Journal of Power Sources 2014, 267, 469-490.Beaulieu, L. Y.; Hatchard, T. D.; Bonakdarpour, A.; Fleischauer, M. D.; Dahn, J. R., Reaction of Li with Alloy Thin Films Studied by In Situ AFM. Journal of The Electrochemical Society 2003, 150 (11), A1457.Hatchard, T. D.; Topple, J. M.; Fleischauer, M. D.; Dahn, J. R., Electrochemical Performance of SiAlSn Films Prepared by Combinatorial Sputtering. Electrochemical and Solid-State Letters 2003, 6 (7), A129.Chen, M., A brief overview of bulk metallic glasses. NPG Asia Materials 2011, 3 (9), 82-90.Jafary-Zadeh, M.; Praveen Kumar, G.; Branicio, P. S.; Seifi, M.; Lewandowski, J. J.; Cui, F., A Critical Review on Metallic Glasses as Structural Materials for Cardiovascular Stent Applications. Journal of Functional Biomaterials 2018, 9 (1), 19.Telford, M., The case for bulk metallic glass. Materials Today 2004, 7 (3), 36-43.Fleischauer, M. D.; Dahn, J. R., Combinatorial Investigations of the Si-Al-Mn System for Li-Ion Battery Applications. Journal of The Electrochemical Society 2004, 151 (8), A1216. Figure 1