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Synthesis of Organo-metallic Coordination Polymers for Thermoelectric Application

Liu, Zilu; (2020) Synthesis of Organo-metallic Coordination Polymers for Thermoelectric Application. Doctoral thesis (Ph.D), UCL (University College London). Green open access

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Abstract

As an intriguing class of thermoelectric (TE) candidates, organometallic coordination polymers (OMCPs) have become a new research focus in this area, regardless of the extensive research on inorganic and organic thermoelectric materials. This thesis showcases the synthesis and comprehensive characterization of a series of linear OMCPs based on metal-bis(dithiolato) coordination, Ni-ett, Ni-diett and Ni-btt (Chapter 2). The studies proved that changing organic ligands is a successful strategy to tune the thermoelectric properties of OMCPs, including electrical conductivity, Seebeck coefficient and power factor. By developing complex model for analogous spectroscopic study, we proved the polymer frames of three OMCPs are radial involving. Moreover, alternative synthetic route was also developed for polymer Ni-btt. Meanwhile, a couple of structural isomeric ligands OMCPs (Chapter 3), benzene-1,2,3,4-tetrakis(thiolate) and benzene-1,2,4,5-tetrakis(thiolate), were employed to synthesize mono-ligand OMCPs (Ni-ibtt and Ni-btt) and dual-ligand OMCPs Ni(ibtt)x(btt)1-x. The comparative study upon their thermoelectric properties was correlated with their structural difference in both intrachain and interchain characters. Regardless of organic bridging ligand, the metal center is the other most important role on the thermoelectric properties of OMCPs. Systematic comparison among OMCPs with different metal centers cross reports is usually unfeasible, as chemical composition and properties for a certain OMCP formula usually (like Ni-ett) differ from ii report to report and involve multiple reaction and measurement factors. In this study, OMCPs with various metal cations were synthesized in the M-ett and M-btt system to conduct a parallel comparison in their thermoelectric performance (Chapter 4). Preliminary molecular design and synthesis work were also carried out to experimentally obtain the OMCPs based on benzenetetrathiolate backbone with different sidechains, to examine the effect of sidechains on thermoelectric properties in this system.

Type: Thesis (Doctoral)
Qualification: Ph.D
Title: Synthesis of Organo-metallic Coordination Polymers for Thermoelectric Application
Event: UCL (University College London)
Open access status: An open access version is available from UCL Discovery
Language: English
Additional information: Copyright © The Author 2020. Original content in this thesis is licensed under the terms of the Creative Commons Attribution 4.0 International (CC BY 4.0) Licence (https://creativecommons.org/licenses/by/4.0/). Any third-party copyright material present remains the property of its respective owner(s) and is licensed under its existing terms. Access may initially be restricted at the author’s request.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10113859
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