In-situ and operando characterization of batteries with energy-dispersive synchrotron x-ray diffraction.

摘要

Batteries play a pivotal role in the low-carbon society that is required to thwart the effects of climate change. Alternative low-carbon energy sources, such as wind and solar, are often intermittent and unreliable. Batteries are able capture their energy and deliver it later when it is needed. The implementation of battery systems in grid-level and transportation sectors is essential for efficient use of alternative energy sources.;Scientists and engineers need better tools to analyze and measure the performance characteristics of batteries. One of the main hindrances in the progress of battery research is that the constituent electrode materials are inaccessible once an electrochemical cell is constructed. This leaves the researcher with a limited number of available feedback mechanisms to assess the cell's performance, e.g., current, voltage, and impedance. These data are limited in their ability to reveal the more-localized smaller-scale structural mechanisms on which the batteries' performance is so dependent.;Energy-dispersive x-ray diffraction (EDXRD) is one of the few techniques that can internally probe a sealed battery. By analyzing the structural behavior of battery electrodes, one is able to gain insight to the physical properties on which the battery's performance is dependent. In this dissertation, EDXRD with ultrahigh energy synchrotron radiation is used to probe the electrodes of manufactured primary and secondary lithium batteries under in-situ and operando conditions. The technique is then applied to solve specific challenges facing lithium ion batteries.;Diffraction spectra are collected from within a battery at 40 micrometer resolution. Peak-fitting is used to quantitatively estimate the abundance of lithiated and non-lithiated phases. Through mapping the distribution of phases within, structural changes are linked to the battery's galvanic response. A three-dimensional spatial analysis of lithium iron phosphate batteries suggests that evolution of inhomogeneity is linked to the particle connectivity. Despite a non-linear local response, the average of the measured ensemble behaves linearly. The results suggest that inhomogeneity can be difficult to measure and highlights the power of the EDXRD technique. Additional applications of EDXRD are discussed.