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Metal-organic materials as electrode precursors and hosts for lithium-ion and lithium-sulfur batteries

Date
2018
Abstract
This thesis describes the development of a range of metal oxide, metal chalcogenide and metal alloy composites, using metal-organic materials (MOMs) as sacrificial precursors and their application as electrode materials in next generation Li-ion batteries. A porous MOM was also implemented as a potential sulfur host in Lithium Sulfur (LiS) batteries. The phase-controlled synthesis of MOM (HKUST-1) derived copper sulfide (CuxS)/C (x = 1, 1.8, 2) composites, via sulfurisation, for the application as cathode materials in Li-ion batteries is described in Chapter 3. This study demonstrates the link between the sulfurisation temperature of the HKUST-1 and the resultant CuxS phase formed with Cu-rich phases formed at higher temperatures. The results indicate the cathode performance is dependent on both the phase of the CuxS and the crystal morphology with the Cu1.8S/C-500 composite with nanowires exhibited the best performance with a specific capacity of 200 mAh/g). Chapter 4 details the synthesis of a new bimetallic 2D interpenetrated MOM and its use as a sacrificial template for the formation of Cu2SnS3/SnS2/C composite and its application as an anode material in Li-ion batteries. The lithiation/delithiation mechanisms of the Cu2SnS3/SnS2/C material were explored as well as the optimisation of the anode testing conditions, leading to the use of a 1 V upper cycling cut-off rather than the conventional voltage limit of 3 V. Cu2SnS3/SnS2/C anodes retained 84 % of their specific capacity after 100 cycles. Chapter 5 explores the synthesis of a range of metal oxide, selenide and alloy composite materials derived from the same MOM precursor demonstrating the versatility of the starting template. This represents the first metal alloy-in-carbon composite from a MOM starting material. Their electrochemical performances are compared with the metal alloy exhibiting the best performance. Chapter 6 details the encapsulation of sulfur within a porous MOM, TIFSIX-1-Cu, for use as a cathode material in LiS batteries. Importantly, the results from the initial electrochemical testing indicate that the interaction between the host material and the electrolyte is very important and demonstrates that a thorough screening process is needed to ensure the stability of the host material prior to sulfur encapsulation and electrochemical testing. TIFSIX-1-Cu interacts with the salts in the electrolyte causing it to be destroyed and meaning that it can no longer act as an effective sulfur host.
Supervisor
Zaworotko, Michael J.
Ryan, Kevin M.
Description
peer-reviewed
Publisher
Citation
Funding code
Funding Information
Science Foundation Ireland (SFI)
Sustainable Development Goals
External Link
Type
Thesis
Rights
https://creativecommons.org/licenses/by-nc-sa/1.0/
License