We report the use of X-ray diffraction in combination with computed tomography to provide quantitative information of a coin cell Li-ion battery and a commercial Ni/MH AAA battery for the first time. This technique allows for structural information to be garnered and opens up the possibility of tracking nanostructural changes in operandi. In the case of the cylindrically wound, standard AAA Ni/MH cell, we were able to map all the different phases in the complex geometry, including anode, cathode, current collector and casing, as well as amorphous phases such as the binder and separator. In the case of a Li-ion coin cell battery, we show how the X-ray diffraction tomography data can be used to map crystal texture of the LiCoO 2 particles over the cathode film. Our results reveal that the LiCoO 2 microparticles show a high degree of preferred orientation, but that this effect is not homogenous over the film, which may affect the electrochemical properties. The design of future energy storage materials relies on an intimate understanding of structural changes occurring as the system operates. While the design of methods for in situ observation of changes in materials is difficult, a number of techniques exist which provide vital information on the physical and chemical transformations occurring in, for example, electrode materials in Li-ion batteries. In situ X-ray diffraction (XRD), 1-4 X-ray absorption spectroscopy (XAS), 2,5,6 X-ray transmission microscopy, 3,7 and Mössbauer spectroscopy 8 have allowed for local electronic and atomic structure determination for a range of candidate materials for Li-ion battery electrodes. However, the continued development of in situ characterization tools is crucial for improving our understanding of the mechanisms governing the performance of batteries.Recently, dynamic X-ray computed tomography (CT) techniques have emerged as an excellent tool for studying microstructural changes and building up a quantitative picture on the scale of particle size. [9][10][11][12] For example, Woo and coworkers have used synchrotron radiation X-ray tomographic microscopy to observe the complex conversion reactions occurring in SnO 2 electrodes, where phase evolution and particle cracking in individual 30 μm-sized particles were observed.
13Wang et al. have also shown that recently developed synchrotron X-ray nanotomography can be applied to tin anodes.14,15 For Li-ion battery research and for smaller commercial applications, coin or button cells are the preferred geometries, and many commercial batteries have a complex spiral wound geometry. However, to date, the CT methods reported have required the design and construction of specialized battery cells. Studies of chemical and structural changes in commercial devices, using spatially resolved, quantitative, non-destructive characterization methods are highly desirable, as this would provide a method to study electrode reactions in situ as realistically as possible. To this end we set out to develop the capability of applying the recently desc...