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Computational Studies of Bulk and Interfacial Properties of Li-ion Battery Anodes

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Abstract:
Energy storage is a crucial aspect of integrating renewable energy sources in power grids, portable electronic devices and vehicle applications, making the development of efficient batteries a high technological challenge. Li ion batteries (LIBs) have been the most important portable power source for consumer electronics and show great promise for vehicle electrification. However, to meet the advanced energy goals required in next-generation vehicular applications, new materials with ultra-high lithium capacities need to be investigated. The study of the bulk and interfacial properties of these new-type electrodes, and especially of their change upon lithiation, is a fundamentally significant and challenging topic in designing heterogeneous nano-structured electrodes for LIBs. This issue becomes more intriguing for silicon (Si) and tin (Sn) electrodes, whose ultrahigh capacity is accompanied by large volumetric expansion and mechanical stresses, having a pivotal impact on the LIBs' performance. Though numerous experiments have been performed to address these issues and trace these changes, in many cases these experimental studies can only report properties that are averaged over time or space, while the local and detailed information of the structure remains buried. Clearly the role of computational studies in acquiring a profound understanding of these mechanisms is critical. Computer simulations at the atomic level, able to provide a unique insight into these changes, can significantly enhance our ability to understand the fundamental interactions between Li ions and the host electrode during Li insertion. Therefore, they can provide a foundation for developing quantitative models for electrode failure and for subsequent development of flaw-tolerant architectures. In this thesis we quantitatively study the lithiation procedure in C, Si and Sn electrodes from first-principles calculations based on density functional theory (DFT) and ab-initio molecular dynamics (AIMD) and study a wide range of different systems and architectures, including surfaces, interfaces and bulk nano-materials. We discuss an assortment of computational aspects related to Li insertion in various types of active host materials, such as bulk Sn, Si/Cu and amorphous Si/C interfaces and introduce the detailed atomistic picture of the lithiation properties and processes from first-principles simulations.
Notes:
Thesis (Ph.D. -- Brown University (2014)

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Citation

Stournara, Maria Eleftheria, "Computational Studies of Bulk and Interfacial Properties of Li-ion Battery Anodes" (2014). Materials Science Engineering Theses and Dissertations. Brown Digital Repository. Brown University Library. https://doi.org/10.7301/Z09W0CT4

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