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2.2 PRD 2 — Link Complex Electronic, Electrochemical, and Physical Phenomena Across Time and Space Over the past decade, much progress has been made in developing and using particle- and photon-based spectroscopy, scattering and imaging techniques, and new modeling frameworks for understanding and predicting mechanisms involved in electrochemical energy storage.1-3 These advances have been achieved largely on a phenomenon-by-phenomenon basis, with each experiment or simulation directed to a particular piece of the electrochemical puzzle, such as lithiation mechanisms, SEI composition, or capacity fade. Connecting the diverse phenomena contributing to battery and electrochemical capacitor operation and failure remains a rich and productive challenge. Understanding coupled phenomena spanning electronic, chemical, structural, and mechanical behavior on the spatial and temporal scales over which they occur is central to moving electrochemical storage from serendipity and trial and error to predictive design. A holistic understanding of electrochemical energy storage devices and deeper insight into the coupling of redox processes, kinetics, reversibility, and degradation phenomena are needed to bring energy storage to the next level. This critical advancement requires the development of more sensitive and accurate multidimensional tools for in situ and operando observation of operating electrochemical systems, new simulation and modeling tools to describe and predict electrochemical outcomes, and greater integration of characterization and modeling. Modeling tools spanning first-principles atomistic to phenomenological mesoscale and continuum levels play increasingly important roles in energy storage research. Density functional theory has significantly advanced the frontier of energy storage materials, both in understanding energy storage phenomena and in predicting new materials by means of high throughput computation. Meanwhile, significant achievements have been made over the past ten years in developing new modeling frameworks to account for the coupling of electrochemical, structural, and mechanical phenomena. The models have been validated by newly developed in situ methods,4 which have allowed these models to be applied for materials invention and optimization within both academia and industry. The new challenge is to link phenomena over a wide range of time and length scales in new models to achieve rational design of batteries as a system. Spectroscopy, scattering, imaging, and electrochemical techniques have seen tremendous advances in the last decade and are the bedrock of energy storage research,5 although at present these techniques are typically used individually. For example, spectro-microscopy has been used to track the reaction dynamics of LiFePO4 electrodes by measuring the relative concentrations of Fe2+ and Fe3+, with the conclusion that nanoscale spatial variations in rate and composition control the lithiation pathway.6,7 While these techniques are fundamental when used individually, there are new horizons of insight attainable by coupling these techniques and the phenomena they probe. Simulation can be similarly coupled and advanced to directly predict measurable experimental outcomes: for example, spectroscopic signatures of reaction pathways, structural degradation on cycling, or SEI formation at interfaces. Overall, the challenge is to develop experiment, simulation, and theory to investigate these coupled phenomena of electrochemical energy storage systems over the full time and length scales on which they occur. NEXT GENERATION ELECTRICAL ENERGY STORAGE PRIORITY RESEARCH DIRECTION – 2 23PDF Image | Next Generation Electrical Energy Storage
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