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Design strategies to enable fast ion transport at metal/solid-electrolyte interfaces is a requirement for solid state batteries, and such strategies must also directly address the substantial influences of volume change, dendrite formation, and metal reactivity. Solid inorganic, polymeric, or ceramic/polymeric composite electrolytes offer synergistic properties, including a high mechanical modulus that can provide a foundation upon which to design electrolytes that overcome these challenges. An additional requirement for stable cell performance is that the interface must be a good ionic conductor and must be mechanically and chemically resilient to changes at the metal electrode during battery operation. 4 3 2 01 4 3 2 1 Emim+ Surface TF2N– 1.5 1.0 0.5 4 03 Surface Layer a Layer b Layer c 00 0 1 2 3 4 5 Separation (nm) 100 nm Figure 2.3.3. Scanning probe microscopy of double layer of the room-temperature ionic [Tf2N-] on graphite. Vertical to the electrode curves reveal the position of individual ion layers (a) which can be mapped revealing set edges as structural defects (b). Imaging of the first ion layer parallel to the electrode surface reveals big domains with layered structural details (c). Courtesy of Nina Balke, Oak Ridge National Laboratory. c 20 40 60 80 x [nm] 10 nm 1.4 1.2 1.0 0.8 0.6 0.4 0.2 0.0 0 LiNi0.5Mn1.5O4 5V LiPON 105 100 95 90 85 80 75 10000 2000 Li 4000 6000 Cycle Number 8000 Figure 2.3.4. Capacity as function of cycle life for Li/LiMn1.5Ni0.5O4 cell with LiPON electrolyte. Reliable cell performance can be obtained with the formation of the right electrode interface. From Ref. 17. Surface the structure of the electric liquid represented as [Emim+] surface, force-distance NEXT GENERATION ELECTRICAL ENERGY STORAGE ab 5 2 1 There are several hypotheses and a small number of theoretical analyses that analyze ion transport and mechanics of the interface; however, none of the predictions has been rigorously validated by experiment. Likewise, several experimental studies allow one to precisely determine how physical and chemical properties of the interface influence battery operation at currents approaching the diffusion-limited value for the electrolyte and interface. It is therefore unclear what sets the maximum current density of the interface reported in experimental studies and what steps might be taken to rationally design the interface to enable high-rate all-solid-state batteries. Currently, it is believed that Li penetrates grain boundaries in polycrystalline solid electrolytes above a few tenths of a mA/cm2 (Figure 2.3.5).18 Why this occurs is currently not understood. As elusive is an understanding of all of the factors that contribute to an observed resistance to dendrite formation at significantly higher current densities for solid electrolytes composed of cross-linked polymers and for conventional liquid electrolytes infused in the pores of nanoporous solid membranes.19,20 Understanding the underlying mechanisms that govern stability of the metal/solid- electrolyte interface and the solid electrolyte is, therefore, a priority for future research. Electrochemical solid-semisolid interfaces, such as electrode-polymer (and gel) electrolyte systems, bridge the behaviors found at solid- liquid and solid-solid interfaces, with gel polymer and solid polymer electrolytes resembling the liquid and solid electrolyte systems, respectively. Polymer-electrolyte-based supercapacitors have demonstrated similar capacitive performance equal to their liquid counterparts.21 However, being a functional “glue” to put all the components together, electrode-polymer electrolyte interfaces can be the “weakest link” as they suffer the most stress during energy storage applications. Understanding these semi-solid interface phenomena not only can enable the applications of polymer electrolytes in many solid energy storage devices but also can facilitate the understanding of solid-solid interfaces. Measuring Electric Potential Distribution across Electrode/Solid-Electrolyte Interfaces: High impedance interfaces are widely believed to represent a major challenge to integrating solid electrolytes with high Li-ion conductivity into practical batteries.22 However, the mechanisms leading to high interfacial impedance remain unclear, in part, because these systems are physically complex, consisting of a variety of electrified materials PRIORITY RESEARCH DIRECTION – 3 41 1st layer 2nd layer 3rd layer 4th layer 5th layer Coulomobic Efficiency (%) Normalized Capacity Count (x 10-3) Force (nN) Separation (nm)PDF Image | Next Generation Electrical Energy Storage
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