Year
2022
Degree Name
Doctor of Philosophy
Department
Institute for Superconducting and Electronic Materials
Abstract
Renewable energy has attracted much attention due to increasing concerns about the sustainability of fossil fuels and environmental issues. Developing sustainable and environmentally friendly ESSs is a great challenge in the 21st century. Lithium-ion batteries (LIBs) have replaced traditional energy storage devices, especially in portable electronic devices and electric vehicles. However, large-scale renewable energy requires low-cost and high-safety energy storage systems and the increasing demands for lithium have brought about the rising costs of lithium resources. Recently, SIBs have been paid significant attention as a promising candidate for large-scale ESSs due to the abundance and low cost of sodium resources. The application of the new synthesis method has prepared new materials, and the defect chemistry of electrode materials has been deeply understood for the first time, which opens up a new route for the design of electrode materials.
Prussian blue analogs are a large family of low-cost transition-metal hexacyanoferrate MOFs with strong structural stability, open 3D structure, and abundant redox-active sites that have been widely studied as electrode materials for both aqueous and nonaqueous SIBs. However, most PBAs suffer from poor cyclability and low Coulombic efficiency due to large lattice distortion during cycling and high vacancies of Fe(CN)6 in crystal frameworks which severely hindered their practical application in high-performance SIBs. Therefore, it is necessary to understand the heterogeneous molecular chemistry in PBAs at the atomic scale and fabricate suitable crystal structures of PBAs to efficiently tackle poor electrochemical properties and side reactions. In this doctoral work, low-cost PBAs (mainly Mn and Fe based) are selected as the investigated target to fabricate high-performance cathodes for SIBs. The main research routes include the designing of novel synthetic methods and the modification of the component inside the crystal structure of the PBAs. Furthermore, the structure-electrochemical performance relationship was systematically investigated through the combination of various characterization methods (including multiple in situ techniques) and theoretical calculations to obtain clear sodium ions storage mechanism and guide the future development and design for the mass production of PBAs for practical energy application.
Recommended Citation
Peng, Jian, Prussian Blue Analogs as Cathode Materials for Sodium-ion Batteries, Doctor of Philosophy thesis, Institute for Superconducting and Electronic Materials, University of Wollongong, 2022. https://ro.uow.edu.au/theses1/1476
FoR codes (2008)
0912 MATERIALS ENGINEERING
Unless otherwise indicated, the views expressed in this thesis are those of the author and do not necessarily represent the views of the University of Wollongong.