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Access Type
WSU Access
Date of Award
January 2023
Degree Type
Dissertation
Degree Name
Ph.D.
Department
Mechanical Engineering
First Advisor
Leela Arava
Abstract
The solid-state battery (SSB) technology holds great promise in large-scale energy storage devices. A few grand challenges, however, such as large interfacial impedance and lower ionic conductivity between the solid-state electrolyte (SSE) and electrodes, are hindering their targeted applications in electric vehicles (EV). The garnet-type cubic Li7La3Zr2O12 (c-LLZO) SSE has generated special attention because of its stability towards lithium-metal anodes, relatively high ionic conductivity, and wide electrochemical stability window. However, achieving target level performance using garnet-type SSE will be nearly impossible without addressing the key issues related to: (i) its high interfacial impedance with metallic lithium due to the poor wetting nature, (ii) its environmental degradation due to the Li+/H+ exchange in the presence of moisture in the atmosphere, (iii) internal short circuit of the battery due to the propagation of lithium dendrites through its grain boundaries and defect sites and (iv) poor mechanical and chemical stability at cathode interface due to volume changes within the cathode. Therefore, a critical challenge in achieving a high performance SSB is the improvement of the interface to ensure high Li+ conductivity between the electrode and electrolyte while facilitating low impedance and high mechanical stability. The hypothesis of this research is that the issues related to electrode/electrolyte interface in SSBs can be resolved by using suitable materials with tailored properties. Materials with high Young’s modulus can suppress the growth of dendrites at the anode-electrolyte interface and accommodate the strain during volume expansion and compression of the cathode. Materials which are hydrophobic in nature can prevent the interaction between moisture and the garnet-type electrolytes, imparting high environmental stability. Also, the material of choice must not hinder lithium ion (Li-ion) transfer across the interfaces. The dissertation research aims at tailoring the electrode/electrolyte interfaces of SSBs by (i) clarifying interfacial reaction mechanisms, (ii) identify and incorporate suitable materials on/in the solid-state electrolyte, (iii) evaluating the interfacial characteristics of modified solid-state electrolytes through electrochemical characterization, (iv) full cell fabrication using LiFePO4 cathodes and lithium metal as the anode for high capacity solid-state battery and (v) probing of the surface/interfacial properties at relevant length scales.
Recommended Citation
Rajendran, Sathish, "Designing Interfaces For All-Solid-State Batteries With Garnet-Type Solid Electrolytes" (2023). Wayne State University Dissertations. 3874.
https://digitalcommons.wayne.edu/oa_dissertations/3874