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This paper1 explores some of the important considerations in devising a practical and consistent framework and methodology for working with experiments and experimental data in connection with modeling and prediction. The paper outlines a pragmatic and versatile “real-space” approach within which experimental and modeling uncertainties (correlated and uncorrelated, systematic and random, aleatory and epistemic) are treated to mitigate risk in modeling and prediction. The elements of data conditioning, model conditioning, model validation, hierarchical modeling, and extrapolative prediction under uncertainty are examined. An appreciation can be gained for the constraints and difficulties at play in devising a viable end-to-end methodology. The considerations and options are many, and a large variety of viewpoints and precedents exist in the literature, as surveyed here. Rationale is given for the various choices taken in assembling the novel real-space end-to-end framework.

Advanced rechargeable lithium-ion batteries are presently being developed and commercialized worldwide for use in consumer electronics, military and space applications. The motivation behind these efforts involves, among other things, a favorable combination of energy and power density. For some of the applications the power sources may need to perform at a reasonable rate at subambient temperatures. Given the nature of the lithium-ion cell chemistry the low temperature performance of the cells may not be very good. At Sandia National Laboratories, we have used different electrochemical techniques such as impedance and charge/discharge at ambient and subambient temperatures to probe the various electrochemical processes that are occurring in Li-ion cells. The purpose of this study is to identify the component that reduces the cell performance at subambient temperatures.

Thermal batteries are normally constructed using pressed-powder anode, separator, and cathode pellets (discs). However, parts less than 0.010” thick are difficult to press from the starting powders. The use of plasma spraying to deposit thin pyrite films onto a stainless steel substrate was examined as an alternative to pressed-powder cathodes. The electrodes were tested under isothermal conditions and constant-current discharge over a temperature range of 400°C to 550°C using a standard LiSi anode and a separator based on the LiCIKCI eutectic. The plasma-sprayed cathodes were also evaluated in similar 5-cell thermal batteries. Cells and batteries using pressed-powder cathodes were tested under the same conditions for comparative purposes.

Silica aerogels have 1/3 the thermal conductivity of the best commercial composite insulations, or ~13 mW/m-K at 25 °C. However, aerogels are transparent in the near IR region of 4-7 μm, which is where the radiation peak from a thermal-battery stack occurs. Titania and carbon-black powders were examined as thermal opacifiers, to reduce radiation at temperatures between 300°C and 600°C, which spans the range of operating temperature for most thermal batteries. The effectiveness of the various opacifiers depended on the loading, with the best overall results being obtained using aerogels filled with carbon black. Fabrication and strength issues still remain, however.