Towards effective electrolyte design for lithium-metal batteries using metal organic frameworks

dc.contributor.advisor Wang, Da-Wei
dc.contributor.advisor Sharma, Neeraj
dc.contributor.advisor Hart, Judy Chua, Stephanie 2022-02-28T05:15:45Z 2022-02-28T05:15:45Z 2021
dc.description.abstract Improvements in liquid lithium-ion battery electrolytes using of metal organic frameworks (MOFs) as a functional decoration on polymer membrane separators were investigated using a combination of experimental and theoretical methods. Zirconium-based MOF UiO-66 was introduced to the polymer support using the mixed matrix membrane (MMM) method. The method allowed the one-step manufacture of a robust, mechanically pliable polymer-MOF membrane composite of high MOF loading. MOF-MMMs imparted improved electrochemical behaviours such as a widened potential operating window, near-unity transference number, and increased presence of solid electrolyte interphase (SEI) components crucial to battery performance. Density functional theory (DFT) calculations were also performed to provide insights regarding electrolyte solvation in the presence of MOF. A simple dip-coating technique was utilised to modify the surface of the MOF-MMMs with polydopamine (PDA) for further improvement of the electrochemical properties. Increased transference numbers, as well as stability during rate cycling, were observed with the resulting PDA-MMM owing to the improved electrode/electrolyte interface. However, surface analyses using x-ray photoelectron spectroscopy (XPS) showed that there are reduced amounts vital SEI components compared to the original MOF-MMM support. The last section further explores the versatility of UiO-66 and tackled the preparation of gel polymer electrolytes (GPEs) decorated with UiO-66 via phase inversion technique. Using the phase inversion method, the fabricated GPE contained pores from both polymer substrate and the intrinsic pores of the 3D nanomaterial for improvement of electrochemical properties. It was demonstrated in this work that the MOF GPE is equally inert and suitable in ether or carbonate-based electrolytes. Overall, this study demonstrated the versatility of UiO-66 metal organic frameworks for use as a functional nanofiller for electrolyte membranes. With the use of inexpensive membrane fabrication methods, the composites obtained are viable for lithium-metal battery applications. Similarly, insights drawn can provide a springboard towards future study of MOF-based electrolytes.
dc.language English
dc.language.iso en
dc.publisher UNSW, Sydney
dc.rights CC BY 4.0
dc.subject.other MOFs
dc.subject.other lithium metal battery
dc.subject.other solid state electrolyte
dc.subject.other UiO-66
dc.subject.other mixed matrix membrane
dc.subject.other gel polymer membrane
dc.title Towards effective electrolyte design for lithium-metal batteries using metal organic frameworks
dc.type Thesis
dcterms.accessRights embargoed access
dcterms.rightsHolder Chua, Stephanie
dspace.entity.type Publication
unsw.accessRights.uri 2024-02-28
unsw.description.embargoNote Embargoed until 2024-02-28
unsw.relation.faculty Engineering
unsw.relation.faculty Science School of Chemical Engineering School of Chemistry School of Materials Science & Engineering School of Chemical Engineering
unsw.subject.fieldofresearchcode 4004 Chemical engineering
unsw.subject.fieldofresearchcode 349999 Other chemical sciences not elsewhere classified
unsw.subject.fieldofresearchcode 401602 Composite and hybrid materials
unsw.thesis.degreetype PhD Doctorate
Resource type