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Ab-Initio Modeling of Degradation Mechanisms in Redox-Flow and Solid-State Batteries

Nadia N Intan, University of Nebraska - Lincoln


The ever increasing energy demand calls for development of energy storage and conversion technologies that can efficiently utilize available renewable energy. In recent years, there has been an immense interest in electrochemically active materials for secondary batteries, most prominently lithium-ion batteries (LIBs) that were developed primarily for portable electronics and now being also used in electric vehicles. At the large scale, redox flow batteries (RFBs) have been attracting increasing attention as stationary energy storage systems that can be connected to an electrical grid and are capable of storing up to hundreds of megawatt-hours of energy. While prior efforts have been predominantly focused on the development of new materials with superior energy characteristics, stability and degradation of electrochemical materials under operation conditions leading to the battery capacity fading have received much less attention. One of the major contributions to the capacity loss in secondary batteries is the formation of passivation layers at the materials interfaces such as electrode/ electrolyte and membrane/electrolyte. Our current atomistic understanding of how chemical reaction dynamics at these interfaces affects capacity fading and the overall battery performance is still limited. The overarching goal of this research project is to provide a better fundamental understanding of this aspect of interfacial chemistry on the example of LIBs and RFBs. Specifically, by employing a combination of density-functional-theory (DFT) based static and molecular dynamics simulations we investigate interfacial behavior focusing on the interactions of: 1) between aqueous electrolyte species and Nafion membrane in all-vanadium RFBs leading to the membrane blockage, and 2) between organic electrolyte species and cathode materials in LIBs leading to electrolyte decomposition and transition-metal dissolution at the interface. By combining the obtained theoretical insights with recent experimental observations, we aim to fill the gap in our microscopic understanding of materials interfacial chemistry leading to detrimental effects in both LIBs and RFBs.

Subject Area

Chemical engineering

Recommended Citation

Intan, Nadia N, "Ab-Initio Modeling of Degradation Mechanisms in Redox-Flow and Solid-State Batteries" (2019). ETD collection for University of Nebraska - Lincoln. AAI27667112.