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REPORT OF THE BASIC RESEARCH NEEDS WORKSHOP and mitigate degradation through the design, synthesis, and intentional incorporation of judiciously selected material interphases into system architectures. To accomplish this, new levels of understanding are needed about the complex processes that control interface formation and evolution — captured in models that can predict the consequences of specific designs and achieved through synthesis that produces the desired structures. Two overarching research thrusts are crucial to realize this vision. First, the complexity of reactive interfaces must be unraveled through experiment and theory. Particular value can be gained from experiments emphasizing spectroscopy and imaging of operating systems to capture the dynamics of interphase formation. X-ray and neutron techniques can have a notable impact as these can penetrate full working cells. Theoretical approaches are needed to treat spatial gradients and their dynamics, with validation of the predictions through relevant experiments. Second, insights so gained must be incorporated into modeling frameworks that enable design of interphases for their desired function. Importantly, the ability to predict and realize new interphase structures opens the door to creative design solutions, e.g., responsive or adaptive membrane separators. ☐ PRD 4 – Revolutionize energy storage performance through innovative assemblies of matter Today’s batteries are based on 2D architectures — stacked layers of anode, electrolyte, and cathode that interact across short inter-layer distances and over large lateral dimensions. New 3D mesoscale architectures are critically needed to tailor performance to diverse applications, allowing the design of the “perfect” battery to match the user’s needs. Among the promising concepts are interdigitated electrodes, where the anode and cathode occupy adjacent “fingers” of the same layer. Nanowire batteries take this interdigitated concept to three dimensions with alternating nanowires of anodes and cathodes interacting across short interwire distances. Fully 3D architectures of adjacent cells, each holding a nanoparticle interacting with neighboring nanoparticles across cell surfaces, are a dramatically new opportunity with significant design flexibility. Flow battery architectures with liquid instead of solid electrodes offer a host of new, alternative design opportunities that have been only marginally explored. Aqueous and non-aqueous electrolytes each offer special appeal, namely, low cost and high operating voltage, respectively. Organic active materials open a rich design space, allowing stability, solubility, and activity to be separately targeted. New possibilities for membranes that only pass desired ions can be based on polymers, glasses, ceramics, or composites. Catalysts afford a rich opportunity to promote targeted energy storage reactions and reduce detrimental side reactions. Semi-flow batteries with one solid and one liquid electrode could allow matching solid and solution- based chemistries in another alternative approach. ☐ PRD 5 – Promote self-healing and eliminate detrimental chemistries to extend lifetime and improve safety The charge and discharge processes that are central to the operation of batteries make them susceptible to gradual degradation that shortens battery life and, on occasion, to catastrophic failure, which is a safety concern. The use of ions for charge storage requires electrode materials to accommodate significant changes such as the stress/strain from volume change, atomic reconfigurations from electrochemical reactions, and localized extremes in temperature, current, and stress. The result is a myriad of unwanted phenomena leading to multiple forms of degradation, including fracture, corrosion, and gas evolution. Understanding and controlling degradation scenarios is a major opportunity for energy storage in the future. Discerning early stages to more clearly illuminate initiating mechanisms is a difficult experimental challenge confounded by the possible presence of multiple degradation initiators. In turn, these initiators may be intrinsic to the battery configuration, may be accelerated by stresses ( e.g., thermal, mechanical, or chemical), or may be simply introduced as manufacturing variations and defects. Current mitigation strategies often result in diminished performance. Correspondingly, the most promising battery chemistries for high performance have been unusable because of accompanying degradation mechanisms. Strategies for both eliminating and mitigating degradation as well as enabling self-healing are needed. Two ambitious research thrusts are proposed to substantially advance the scientific understanding of degradation. First, experiments on operating batteries are needed to quantify degradation and failure, particularly measurements that provide dynamic imaging of the degradation process. When simultaneous electrochemical and materials characterizations are incorporated, these operando experiments can elucidate the causal relationships responsible for degradation. Second, continuum models are required to describe and predict a spectrum of degradation and failure scenarios. The challenge is to model chemical, electrochemical, mechanical, and thermal phenomena dynamically across multiple length scales, translating an understanding at the nanoscale through its manifestations at the macroscale in battery components and cell design. 6 INTRODUCTIONPDF Image | Next Generation Electrical Energy Storage
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