Shutt, Rebecca Roisin Christine;
(2025)
An Investigation of Electrode Nanostructuring in Energy Storage Applications.
Doctoral thesis (Ph.D), UCL (University College London).
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Abstract
Enormous increases in demand for electrochemical energy storage from battery technologies is expected over the forthcoming decades. The research of anode materials for rechargeable, secondary-ion batteries is important to develop new high-performance devices, and of particular significance for sodium ion batteries, for which graphite has a limited reversible capacity. Investigating nanostructuring in anodes can both develop new materials for battery applications and improve our understanding of the storage mechanisms governing electrochemical performance. This thesis aims to investigate the role of nanostructuring materials for battery anodes targeting both recently-isolated phosphorene nanoribbons (PNRs) tested as novel active materials for lithium ion batteries, and the lithiation/sodiation mechanisms within hard carbon using neutron scattering. Previously restricted to protective coatings on lithium metal anodes, recently-isolated PNRs were successfully applied as an anode material with carbon black. The electrodes achieved reversible lithiation capacities of up to 160 mAh g–1 with limited capacity degradation after 80 cycles. Pioneering total neutron scattering studies were completed on hard carbon electrodes during (operando) and post- (ex situ) electrochemical cycling, characterising lithium- and sodium ion systems. Neutron total scattering enabled the simultaneous characterisation of the nanoporosity and the turbostratic nanodomains, providing a powerful tool for analysis of the “closed” porosity, for which other characterisation techniques are insufficient. An expansion of the spacing between graphene layers in the turbostratic nanodomains (TNDs) from 0.38 nm to up to 0.42 nm was detected along with an accompanying narrowing of the full-width half-maximum. Contrast differences observed between the nanopores and TNDs at low voltage could only be explained through the occupation of the lithium and sodium ions in the nanopores, supporting the intercalation-first-before-pore-filling mechanism.This thesis aims to investigate the role of nanostructuring materials for battery anodes targeting both recently-isolated phosphorene nanoribbons (PNRs) tested as novel active materials for lithium ion batteries, and the lithiation/sodiation mechanisms within hard carbon using neutron scattering. Previously restricted to protective coatings on lithium metal anodes, recently-isolated PNRs were successfully applied as an anode material with carbon black. The electrodes achieved reversible lithiation capacities of up to 160 mAh g–1 with limited capacity degradation after 80 cycles. Pioneering total neutron scattering studies were completed on hard carbon electrodes during (operando) and post- (ex situ) electrochemical cycling, characterising lithium- and sodium ion systems. Neutron total scattering enabled the simultaneous characterisation of the nanoporosity and the turbostratic nanodomains, providing a powerful tool for analysis of the “closed” porosity, for which other characterisation techniques are insufficient. An expansion of the spacing between graphene layers in the turbostratic nanodomains (TNDs) from 0.38 nm to up to 0.42 nm was detected along with an accompanying narrowing of the full-width half-maximum. Contrast differences observed between the nanopores and TNDs at low voltage could only be explained through the occupation of the lithium and sodium ions in the nanopores, supporting the intercalation-first-before-pore-filling mechanism.
| Type: | Thesis (Doctoral) |
|---|---|
| Qualification: | Ph.D |
| Title: | An Investigation of Electrode Nanostructuring in Energy Storage Applications |
| Open access status: | An open access version is available from UCL Discovery |
| Language: | English |
| Additional information: | Copyright © The Author 2025. Original content in this thesis is licensed under the terms of the Creative Commons Attribution-NonCommercial 4.0 International (CC BY-NC 4.0) Licence (https://creativecommons.org/licenses/by-nc/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 Engineering Science > Dept of Chemical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10203198 |
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