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Improved reaction mechanism. Even the more detailed multi-step reaction mech- anism does not include all possible reactions in the Li/S cell. In fact, the inclusion of every possible effect is not an end in itself – approximations, simplifications, and exclusions are an essential part of every decent model. However, at least the addition of disproportionation reactions as well as a more detailed description of precipitation and dissolution are considered critical tasks. As discussed above, Refs. [44, 142, 264] provide a good starting point for formulating a revised reaction mechanism, fully supported by experiments. Microstructure. While a full 3D model is beyond the scope and besides the purpose of our modeling activities, the parametrization could be improved by simulating rep- resentative elements of an electrode in full 3D or by analyzing the structure in other ways in order to obtain more accurate effective parameters. An approach similar to Refs. [270, 271] could be followed, using SEM, FIB-SEM, or TEM images to establish a realistic microstructure layout as a base for the computation of effective transport parameters and active surface areas as outlined in Ref. [272]. Degradation. Many more chemical degradation mechanisms may be added to the model in a straightforward fashion, ranging from simple parasitic reactions like sol- vent oxidation to a full SEI model in the style of Refs. [273–275]. Additionally, one can think of non-chemical degradation mechanisms such as mechanical deformation [276], cracking [218], agglomeration, or the build-up of insulating layers [277]. All of these directly affect the transport in the cell, but can also result in loss of electric con- tact in parts of the porous cathode [278]. However, lacking systematical studies on the degradation effects, it would be difficult to determine the right reaction mechanism(s) and parameters for even more side reactions. On the other hand, a first systematical and methodologically sound experimental analysis of the polysulfide shuttle has been published recently by Janek et al. [279], which might enable a better parametrization and hence more realistic simulation of this particular parasitic reaction in the future. Transport in the liquid electrolyte. First of all, a more detailed description of the ionic liquid is required in order to improve the modeling of transport in the liquid electrolyte. Another interesting improvement would be the description of locally non- neutral concentrated electrolytes [207], potentially built on top of a thermodynamically consistent description of the ionic transport in liquid electrolytes [203]. The latter would also pave the way for a theoretically sound temperature-dependent model of the Li/S battery, outlined next. 135PDF Image | Lithium-Sulfur Battery: Design, Characterization, and Physically-based Modeling
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