2015
DOI: 10.1021/jp510882g
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Abstract: A central challenge in the refinement of lithium-ion batteries is to control cathode-induced oxidative decomposition of electrolyte solvents, such as ethylene carbonate (EC) and dimethyl carbonate (DMC). We study the oxidation potentials of neat EC, neat DMC, and 1:1 mixtures of EC and DMC using the newly developed projection-based embedding method, which we demonstrate to be capable of correcting qualitative inaccuracies in the electronic densities and ionization energies obtained from conventional Kohn−Sham … Show more

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Cited by 53 publications
(68 citation statements)
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“…59 The approach is implemented in the widely used Molpro software package, 60 allowing straightforward application of projection-based WF-in-DFT embedding for quantum chemical studies. 58,65,[67][68][69][70][71][72][73][74][75][76][77][78][79][80] Looking forward, we anticipate continued refinement of the projection-based embedding methodology, as well as increasingly widespread application in diverse areas of chemistry, biology, and materials science.…”
Section: Outlook and Conclusionmentioning
confidence: 99%
“…59 The approach is implemented in the widely used Molpro software package, 60 allowing straightforward application of projection-based WF-in-DFT embedding for quantum chemical studies. 58,65,[67][68][69][70][71][72][73][74][75][76][77][78][79][80] Looking forward, we anticipate continued refinement of the projection-based embedding methodology, as well as increasingly widespread application in diverse areas of chemistry, biology, and materials science.…”
Section: Outlook and Conclusionmentioning
confidence: 99%
“…Adaptive QM/MM simulations are especially well suited for this problem, as they allow for flexible description of solvent/ion interactions and the forced localization of redox processes within the QM region. This not the first QM/MM approach to the lithium battery electrolytes, but our codes feature the first framework of its kind . The following two examples are designed to illustrate these features.…”
Section: Running Simulationsmentioning
confidence: 99%
“…This approach, with some slight modifications, has been applied successfully to a wide range of chemical problems. [24][25][26][27][28] Although the projection-based embedding has already seen significant successes, its use as a "black box" method presents some challenges. The Mulliken charge threshold employed in the partition of the A and B orbital subspaces is rather arbitrary, while the very concept of Mulliken charge can have deleterious effects, as it does not have a basis set limit and is not always in accordance with well-established chemical intuition backed by empirical evidence.…”
Section: Introductionmentioning
confidence: 99%