Abstract
Electrolyte formulations in standard lithium ion and lithium metal batteries are complex mixtures of various components. In this article, we review molecular key principles of ion complexes in multicomponent electrolyte solutions in regards of their influence on charge transport mechanisms. We outline basic concepts for the description of ion–solvent and ion–ion interactions, which can be used to rationalize recent experimental and numerical findings concerning modern electrolyte formulations. Furthermore, we discuss benefits and drawbacks of empirical concepts in comparison to molecular theories of solution for a more refined understanding of ion behavior in organic solvents. The outcomes of our discussion provide a rational for beneficial properties of ions, solvent, co-solvent and additive molecules, and highlight possible routes for further improvement of novel electrolyte solutions.
Highlights
The use of multicomponent electrolyte solutions in modern electrochemical storage devices such as rechargeable lithium ion and lithium metal batteries (LIBs and LMBs) is of fundamental importance for effective ion shuttling and transport mechanisms [1,2,3,4,5,6,7,8,9,10]
The question arises: How can the presence of co-solvent molecules induce a change of ion correlation effects? With regard to our previous discussion in Section 3, it can be assumed that local interactions between the co-solvent molecules and the ions are mainly responsible for the observed variations
The outcomes of several studies discussed in this article highlight that most processes in organic solvent-based electrolyte solutions are very complex
Summary
The use of multicomponent electrolyte solutions in modern electrochemical storage devices such as rechargeable lithium ion and lithium metal batteries (LIBs and LMBs) is of fundamental importance for effective ion shuttling and transport mechanisms [1,2,3,4,5,6,7,8,9,10]. The development of novel electrolyte formulations often relies on limited molecular understanding, empirical arguments, theoretical approaches suffering from unspecific approximations, or previous experimental findings instead of a desirable frame-guided design of tailor-made components for distinct purposes. In this context, refined theoretical and numerical approaches often provide useful frameworks to establish a more advanced level of understanding.
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