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of structural defects/vacancies and the disorder that often accompanies this blended capacitor/battery behavior. Such materials are often difficult to characterize by conventional methods that rely on crystallinity/structural periodicity. However, newer tools using synchrotron-based techniques offer the promise of unraveling the structural complexity of poorly ordered or defective materials that otherwise display intriguing charge-storage characteristics.87 Ex situ characterization will provide baseline information on material structure, but the ability to perform such measurements in situ or operando will be critical in elucidating the charge-storage mechanisms that may be at play in such systems. Further, because the materials in question will support electrochemical processes occurring on the order of a few seconds, the tools used to characterize them must be able to measure dynamically at such time scales. Advanced characterization should also be coupled with computation/modeling of such solid-state structures. Modeling of pseudocapacitors is still in its infancy. There are currently no good models to describe these materials due to the complexity of the interfacial physical chemistry. There are multiple considerations here as the surface structure, surface reaction pathway, reaction kinetics, overpotential, solvent effect, and electrolyte pH are all able to greatly influence pseudocapacitive behavior, which is characterized by surface redox reactions. It is likely that a multi-scale approach is necessary. Moreover, modeling at the microstructural level should assist in directing the design of porous electrode architectures that deliver high capacity/energy, but on supercapacitor-like time scales. Design Effective Electrodes, Electrolytes, and Interfaces: Understanding how densely packed solids facilitate the motion of positively charged ions through their lattices is crucial for accelerating the design of next generation intercalation hosts and solid electrolytes that can transport next generation elements like Na or multivalent cations. This is particularly challenging for materials consisting of compositions with a mixture of rigid covalent and more flexible ionic bonds, as in polyanionic compounds.88,89 These structural deformations are not only critical for influencing the rate of ionic diffusion, but also have direct consequences for the mechanical properties and the potential for particle fracture over extended cycling. Developing better experimental and computational methods to characterize the nature of cooperative structural distortions is an area that would greatly facilitate the prediction of local stresses that can build inside the intercalation hosts during (de)insertion while simultaneously building the fundamental understanding of how to accelerate the transport of ions through materials. Superconcentrated electrolytes are destined to emerge as a vital factor in advancing electrochemical energy storage. This is because specific solution structures (both bulk and at electrode/electrolyte interfaces) associated with these chemistries may have great beneficial impact on the mitigation of unwanted reactions that cause major safety problems in batteries. This field of electrolytes has received only a limited amount of study. The opportunity here is to integrate data mining with advanced atomic-scale simulations and in situ high-level characterization, which can then be used to guide experimental studies directed at structure/property relations. A key issue to be considered with these electrolytes, both computationally and experimentally, is their unique solvation properties, which can then be used to provide new chemical insights. A well-defined challenge with these studies will be to extract design rules from a vast chemical space for electrolyte design and development. Ionogels present a tantalizing opportunity in which to achieve liquid-like ion transport and interfacial transport in a solid-state matrix. Their incorporation in solid-state batteries can be transformative to this technology if the presence of the local liquid phase produces a low interfacial resistance, as occurs in liquid electrolyte systems. This may result in extended battery lifetimes. Moreover, designing appropriate mesoporous host matrices may yield materials with reduced dimensionality and with confined liquid phases that can operate at low temperatures. Making the Use of Li Metal Anodes a Reality: There is a critical need for improved operando analysis of Li metal anodes, which will increase our understanding of the coupled electrochemical, morphological, and mechanical behavior of the negative electrode and its interface. Combining experimental work with multi-scale modeling will enable the research community to move towards experimentally informed design, and away from empirical approaches based on qualitative or semi-quantitative concepts. One of the most important challenges is to develop a tailored solid-electrolyte interphase for the high-volume-change Li-alloy materials. Some of the basic scientific questions that need to be addressed are: What are the origins of the spatial/temporal variations in chemical composition and impedance of the solid-electrolyte interphase during cycling? What are the chemical NEXT GENERATION ELECTRICAL ENERGY STORAGE PANEL 4 REPORT 123PDF Image | Next Generation Electrical Energy Storage
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