New Multi-Scale Simulation Methods for Understanding and Mitigating Dendrite Growth and electrolyte Decomposition in Rechargeable Lithium Metal Batteries
Abstract
Funds are provided to extend prior theoretical models developed for chemical electrodeposition to understand the fundamental mechanisms associated with the formation of lithium dendrites and the solid electrolyte interphase in lithium batteries to provide significant new insight into molecular processes and material properties. Future energy storage needs for naval, automotive, and aerospace applications pose unique battery challenges related to capacity, lifetimes, and thermal ranges. Beyond state-of-the-art lithiumion technologies, there is an urgent need for advances in the energy density, power density, stability, and safety of battery systems. We propose the extension and application of a multi-scale simulation approach to understand and prevent dendrite formation in rechargeable lithium metal batteries. Batteries that utilize lithium metal for the anode material offer unparalleled energy density and promise new technologies and applications. However, rechargeable lithium batteries are plagued by the formation of needle-like lithium dendrites during anodal electrodeposition, causing battery failure. Understanding the molecular processes and interactions that govern lithium electrodeposition is essential for the design of methods and materials to inhibit or prevent dendrite formation. The multi-lengthscale, heterogeneous, and non-equilibrium nature of lithium electrodeposition poses extraordinary challenges for experimental and computational analysis. To address this challenge, the Miller group has employed ONR funding to develop a simulation strategy that combines both top-down (i.e., coarse-grained) and bottom-up (i.e., atomistic) approaches to modeling chemical electrodeposition. We propose to extend this combined strategy to (i) to elucidate the fundamental mechanisms associated with the formation of both lithium dendrites and the solid electrolyte interphase (SEI) via electrolyte decomposition, and (ii) to discover electrolyte materials and deposition conditions that inhibit dendrite formation at lithium-metal anodes for ONR-relevant battery applications. This work will provide direct insight into the molecular processes and material properties that govern battery lifetime, charging/discharging rates, and SEI properties for both current and next-generation battery systems. Specific Aim 1: Coarse-grained modeling of dendrite formation. We propose to extend coarsegrained models that capture the essential physics of lithium deposition and dendrite formation in a rechargeable battery. These models allow for direct, non-equilibrium simulations that span the long timescales and lengthscales associated with the dynamics of dendrite formation. We will develop understanding of the competing kinetic and thermodynamic processes that govern lithium dendrite formation, and we will identify materials and approaches to mitigate dendrite formation. Specific Aim 2: Fundamental studies of early stage solid electrolyte interphase (SEI) formation and Li anode reaction chemistry. We propose to use detailed atomistic simulations to investigate the key interactions, statistical mechanical properties, and reaction mechanisms and dynamics associated with lithium dendrite formation and electrolyte decomposition and stability. Scientific merit and relevance to ONR interests. The proposed research addresses an area of primary naval research interest and a challenge that is at the forefront of basic energy scientific research. By elucidating the molecular mechanism of dendrite formation, the proposed research will yield breakthrough design strategies and new materials for the development of viable, rechargeable lithium metal batteries.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Nov 23, 2016
- Source ID
- N000141612761
Entities
People
- Thomas M Miller
Organizations
- California Institute of Technology
- Office of Naval Research
- United States Navy