In spite of its technological relevance in the energy conversion andstorage, our knowledge about the microscopic structure ofelectrochemical electrode-electrolyte interfaces is still ratherlimited. This is particularly true for electrochemical interfacesin batteries which typically exhibit an ill-defined structure.In this contribution, we will present our attempts to contribute to to a deeper understanding based on electronic structure calculationsby systematically increasing the complexity of the considered systems.We will discuss the surface structures of both anode and cathodematerials.  Ionic compounds that are often used as electrode materialsin Li-based rechargeable batteries can exhibit polar surfaces whichare generally accepted to exhibit rather large surface energies.  Wehave recently derived a scheme to estimate the polar contribution tothe surface energy [1]. Due to a polarity compensation mechanism polarsurface can still be rather stable, as we show using lithium-ironsilicate as an example. Furthermore, we address the structure of metallicelectrodes and their interaction with ionic charge carriers [2].In addition, we discuss the influence of the electrolyte usingboth implicit and explicit solvent models.References[1] N. Hoermann and A. Gross, ChemPhysChem, accept. for publ.[2] F. Gossenberger, T. Roman, K. Forster-Tonigold, and Axel Gross,  Beilstein J. Nanotechnol. 2014, 5, 152-161.

First-principles modeling of electrochemical interfaces for energy storage

248th National Meeting (2014)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.