Abstract
The electrochemical stability vs. oxidation is a crucial property of anions in order to be suitable as components in lithium-ion batteries. Here the applicability of a number of computational approaches and methods to assess this property, employing a wide selection of DFT functionals, has been studied using the CCSD(T)/CBS method as the reference. In all, the vertical anion oxidation potential, ΔEv, is a fair way to calculate the stability vs. oxidation, however, a functional of at least hybrid quality is recommended. In addition, the chemical hardness, η, is identified as a novel approach to calculate the stability vs. oxidation.
Highlights
Electrolytes are a key component of batteries and their electrochemical stability windows (ESWs); the potential range wherein none of its components breaks down due to oxidation or reduction, currently limit the capabilities of Li-ion batteries (LIBs).[1]
As MP2 energies are included in the results of the CCSD(T) calculations, the anions in Table 1 can function as an internal benchmark for the DCBS method
For the calculation of the stability vs. oxidation for the present set of anions, using the methodology of DEv, a hybrid functional is recommended. Their resulting DEv values are closer to the benchmark, surpassing the previously recommended VSXC functional of older works.[26,27]
Summary
Electrolytes are a key component of batteries and their electrochemical stability windows (ESWs); the potential range wherein none of its components breaks down due to oxidation or reduction, currently limit the capabilities of Li-ion batteries (LIBs).[1] This is due to the high voltages possible for LIBs, often above 4 V. As there is a strong desire to produce even higher voltage cathodes,[2] to allow for even higher energy density LIBs – a very high oxidation stability (preferably 45 V vs Li+/Li) is aimed at for future electrolytes. In order to reduce trial-and-error efforts, tools to predict electrochemical stability from chemical structure alone are of large interest. One way is by in silico screening, which allows for rapid evaluation of candidates for future synthesis
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