Publications Details

Real-time Studies of Battery Electrochemical Reactions Inside a Transmission Electron Microscope

Sullivan, John P.; Huang, Jian Y.; Leung, Kevin; Shaw, Michael; Fan, Hongyou; Liu, Xiaohua L.; Liu, Yang; Hudak, Nicholas S.

We report the development of new experimental capabilities and ab initio modeling for real-time studies of Li-ion battery electrochemical reactions. We developed three capabilities for in-situ transmission electron microscopy (TEM) studies: a capability that uses a nanomanipulator inside the TEM to assemble electrochemical cells with ionic liquid or solid state electrolytes, a capability that uses on-chip assembly of battery components on to TEM-compatible multi-electrode arrays, and a capability that uses a TEM-compatible sealed electrochemical cell that we developed for performing in-situ TEM using volatile battery electrolytes. These capabilities were used to understand lithiation mechanisms in nanoscale battery materials, including SnO₂, Si, Ge, Al, ZnO, and MnO₂. The modeling approaches used ab initio molecular dynamics to understand early stages of ethylene carbonate reduction on lithiated-graphite and lithium surfaces and constrained density functional theory to understand ethylene carbonate reduction on passivated electrode surfaces.