Publication:
Computer-Guided Design of Photocatalyst for PET-RAFT Polymerisation
Computer-Guided Design of Photocatalyst for PET-RAFT Polymerisation
dc.contributor.advisor | Boyer, Cyrille | en_US |
dc.contributor.advisor | Xu, Jiangtao | en_US |
dc.contributor.author | Wu, Chenyu | en_US |
dc.date.accessioned | 2022-03-15T12:47:24Z | |
dc.date.available | 2022-03-15T12:47:24Z | |
dc.date.issued | 2020 | en_US |
dc.description.abstract | Photo-controlled polymerisation uses a photo-excited photocatalyst (PC) to reversibly and deactivate the propagating species. Under regulation by light, photo-controlled polymerisation features temporal control, spatial control, sequence control and high level of selectivity/orthogonality between different systems, leading to a range of applications in advanced macromolecular synthesis such as surface patterning, 3D/4D printing, polymeric micelles, multiblock antimicrobial polymers with precise sequences and architectures. All these unique features of photo-controlled polymerisation are largely dependent on properties and functionalities of PCs. Traditionally, the selection and discovery of appropriate PCs rely heavily on a trail-and-error approach, where extensive experimental screening is needed to identify desired candidates. To reduce costs and circumvent the challenges in laborious experimental work, a rational design strategy emerged where a new PC in application to a photo-controlled polymerisation system can be designed based on understanding of the structure-property-performance relationships. This dissertation aims to enable and streamline a general fully computer-guided rational strategy of designing an efficient and functional PC for a commonly used photocontrolled polymerisation technique, namely photoinduced electron/energy reversible addition-fragmentation chain transfer (PET-RAFT) polymerisation. This thesis starts from using naturally evolved Chl a with various functional substituents and investigating its photocatalytic performance and functionalities in PET-RAFT polymerisation. General orientations for the design of PET-RAFT PCs were inspired from this natural design. On top of this, comprehensive structure-property-performance relationships were established at the quantum chemical level as guiding principles for rational PC design of PET-RAFT polymerisation, by combining experimental and computational studies on a library of halogenated xanthene dyes. Finally, by implementing the most cutting-edged quantum chemical software packages, the fully computer-guided strategy of functional PC design for PET-RAFT polymerisation was enabled based on broadened structure-property-performance relationships. As an example, an efficient pH-switchable organic PC was designed. Application of this rationally designed PC in PET-RAFT polymerisation resulted in the first organocatalysed pH and light dual-gated controlled polymerisation. | en_US |
dc.identifier.uri | http://hdl.handle.net/1959.4/68278 | |
dc.language | English | |
dc.language.iso | EN | en_US |
dc.publisher | UNSW, Sydney | en_US |
dc.rights | CC BY-NC-ND 3.0 | en_US |
dc.rights.uri | https://creativecommons.org/licenses/by-nc-nd/3.0/au/ | en_US |
dc.subject.other | Photopolymerisation | en_US |
dc.subject.other | Polymerisation | en_US |
dc.subject.other | Photocatalysis | en_US |
dc.subject.other | Photocatalyst | en_US |
dc.subject.other | Photocatalyst design | en_US |
dc.subject.other | PET-RAFT | en_US |
dc.subject.other | Radical polymerisation | en_US |
dc.subject.other | PC design | en_US |
dc.subject.other | Functional photocatalyst | en_US |
dc.title | Computer-Guided Design of Photocatalyst for PET-RAFT Polymerisation | en_US |
dc.type | Thesis | en_US |
dcterms.accessRights | open access | |
dcterms.rightsHolder | Wu, Chenyu | |
dspace.entity.type | Publication | en_US |
unsw.accessRights.uri | https://purl.org/coar/access_right/c_abf2 | |
unsw.date.embargo | 2021-07-01 | en_US |
unsw.description.embargoNote | Embargoed until 2021-07-01 | |
unsw.identifier.doi | https://doi.org/10.26190/unsworks/3949 | |
unsw.relation.faculty | Engineering | |
unsw.relation.originalPublicationAffiliation | Wu, Chenyu, Centre for Advanced Macromolecular Design, Faculty of Engineering, UNSW | en_US |
unsw.relation.originalPublicationAffiliation | Boyer, Cyrille, Centre for Advanced Macromolecular Design, Faculty of Engineering, UNSW | en_US |
unsw.relation.originalPublicationAffiliation | Xu, Jiangtao, Centre for Advanced Macromolecular Design, Faculty of Engineering, UNSW | en_US |
unsw.relation.school | School of Chemical Engineering | * |
unsw.thesis.degreetype | PhD Doctorate | en_US |
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