Cell design and image analysis for in situ Raman mapping of inhomogeneous state-of-charge profiles in lithium-ion batteries

The study of inhomogeneous battery failure processes requires proper tools with high spatial resolving power. Here we describe a simple way to adapt industry-standard coin cells to enable in situ Raman mapping of lithium-ion battery materials. We describe the important cell design parameters and validate that the design achieves a uniform potential distribution within the region probed by Raman. We further validate that the cell yields electrical performance characteristics equivalent to a standard, non-modified coin cell. Using this cell, we probe the local charging profiles of LiNi0.5Mn0.3Co0.2O2 (NMC) particles during cycling and demonstrate the ability to achieve spatial maps of the Raman spectra. In order to reduce the effects of local topography, we further analyze these data by numerically extracting the local frequency of the A1g vibrational mode, which is sensitive to the local extent of lithiation, and producing spatial maps of the local frequency of the A1g mode. This work demonstrates a way to collect and analyze high quality in situ spectra with an easy-to-implement cell design that can be applied to a wide range of electrode materials. (C) 2017 Published by Elsevier B.V.