Mechanical degradation and resultant capacity fade in high-capacity electrode materials critically hinder their use in high-performance rechargeable batteries. Despite tremendous efforts devoted to the study of the electro–chemo–mechanical behaviours of high-capacity electrode materials, their fracture properties and mechanisms remain largely unknown. Here we report a nanomechanical study on the damage tolerance of electrochemically lithiated silicon. Our in situ transmission electron microscopy experiments reveal a striking contrast of brittle fracture in pristine silicon versus ductile tensile deformation in fully lithiated silicon. Quantitative fracture toughness measurements by nanoindentation show a rapid brittle-to-ductile transition of fracture as the lithium-to-silicon molar ratio is increased to above 1.5. Molecular dynamics simulations elucidate the mechanistic underpinnings of the brittle-to-ductile transition governed by atomic bonding and lithiation-induced toughening. Our results reveal the high damage tolerance in amorphous lithium-rich silicon alloys and have important implications for the development of durable rechargeable batteries.
Germanium (Ge) is a promising candidate anode material for next-generation, high-performance lithium-ion batteries. Despite its apparent promise, the mechanical properties of lithiated Ge including its fracture characteristic are largely unknown. In this paper, we report the first experimental measurement of the fracture toughness of lithiated Ge using an in-house developed nanoindentation system. The fracture toughness of lithiated Ge is found to increase monotonically with increasing lithium content, indicating a brittle-to-ductile transition of lithiated Ge as lithiation proceeds. We also compare the fracture energy of lithiated Ge with that of lithiated Si and show that, despite a slightly lower fracture energy of Ge than that of Si in the unlithiated state, Ge possesses much higher fracture resistance than Si in the lithiated state. These findings suggest that Ge anodes are intrinsically more resistant to fracture than their Si counterparts, thereby offering substantial potential for the development of durable, high-capacity, and high-rate lithium-ion batteries. The quantitative results from this work provide fundamental insights for developing new electrode materials and help to enable predictive modeling of high-performance lithium-ion batteries. Rechargeable lithium-ion batteries (LIBs) are the current dominant energy storage solution for portable electronics and electric vehicles. The growing demand in these applications, however, requires next-generation LIBs with an unprecedented combination of low cost, high capacity, and high reliability. To significantly enhance the LIB performance, much of the research effort to date has been devoted to developing new electrode materials that can store more Li ions than the current available technology. In today's commercial LIBs, graphite of 372 mAhg −1 capacity is being widely used as the anode material.
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