{"id":{"repo_id":"unsw","oai_identifier":"oai:unsworks.library.unsw.edu.au:1959.4/68278"},"canonical_url":"https://search.dev.ndltd.org/etd/unsw/oai:unsworks.library.unsw.edu.au:1959.4/68278","repository":{"repo_id":"unsw","name":"University of New South Wales","base_url":"https://unsworks.unsw.edu.au/oai/provider"},"display":{"title":"Computer-Guided Design of Photocatalyst for PET-RAFT Polymerisation","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.","abstract_html":"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.","abstract_has_math":false,"creators":["Wu, Chenyu"],"institution":"UNSW, Sydney","degree_name":null,"degree_level":null,"degree_discipline":null,"degree_department":null,"school":null,"contributors":[],"advisors":[],"committee_chairs":[],"committee_members":[],"year":2020,"date_issued":"2020","date_published":"2020","updated_at":"2026-07-24T05:32:27Z","subjects":["Photopolymerisation","Polymerisation","Photocatalysis","Photocatalyst","Photocatalyst design","PET-RAFT","Radical polymerisation","PC design","Functional photocatalyst"],"languages":["EN"],"rights":["open access","CC BY-NC-ND 3.0","free_to_read"],"rights_urls":["https://purl.org/coar/access_right/c_abf2","https://creativecommons.org/licenses/by-nc-nd/3.0/au/"],"identifier_entries":[{"key":"dc:identifier","label":"Identifier","values":["https://doi.org/10.26190/unsworks/3949"],"render_values":[{"text":"https://doi.org/10.26190/unsworks/3949","href":"https://doi.org/10.26190/unsworks/3949","code":true}]}]},"links":{"outbound_url":"http://hdl.handle.net/1959.4/68278","outbound_label":"Handle","outbound_source":"dc:identifier"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:creator","label":"Author","values":["Wu, Chenyu"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:date","label":"Dc Date","values":["2020"]},{"key":"dc:publisher","label":"Institution","values":["UNSW, Sydney"]},{"key":"dc:type","label":"Dc Type","values":["doctoral thesis","http://purl.org/coar/resource_type/c_db06"]}]},{"id":"subjects_keywords","label":"Subjects and Keywords","entries":[{"key":"dc:subject","label":"Dc Subject","values":["Photopolymerisation","Polymerisation","Photocatalysis","Photocatalyst","Photocatalyst design","PET-RAFT","Radical polymerisation","PC design","Functional photocatalyst"]}]},{"id":"language_rights","label":"Language and Rights","entries":[{"key":"dc:language","label":"Dc Language","values":["EN"]},{"key":"dc:rights","label":"Dc Rights","values":["open access","https://purl.org/coar/access_right/c_abf2","CC BY-NC-ND 3.0","https://creativecommons.org/licenses/by-nc-nd/3.0/au/","free_to_read"]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier","label":"Identifier","values":["http://hdl.handle.net/1959.4/68278","https://unsworks.unsw.edu.au/bitstreams/743100cc-115d-4f8b-b012-cb72796f9efe/download","https://doi.org/10.26190/unsworks/3949"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description","label":"Description","values":["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."]},{"key":"dc:format","label":"Dc Format","values":["application/pdf"]},{"key":"dc:title","label":"Title","values":["Computer-Guided Design of Photocatalyst for PET-RAFT Polymerisation"]}]}],"canonical_facts":{"dc:creator":["Wu, Chenyu"],"dc:date":["2020"],"dc:description":["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."],"dc:format":["application/pdf"],"dc:identifier":["http://hdl.handle.net/1959.4/68278","https://unsworks.unsw.edu.au/bitstreams/743100cc-115d-4f8b-b012-cb72796f9efe/download","https://doi.org/10.26190/unsworks/3949"],"dc:language":["EN"],"dc:publisher":["UNSW, Sydney"],"dc:rights":["open access","https://purl.org/coar/access_right/c_abf2","CC BY-NC-ND 3.0","https://creativecommons.org/licenses/by-nc-nd/3.0/au/","free_to_read"],"dc:subject":["Photopolymerisation","Polymerisation","Photocatalysis","Photocatalyst","Photocatalyst design","PET-RAFT","Radical polymerisation","PC design","Functional photocatalyst"],"dc:title":["Computer-Guided Design of Photocatalyst for PET-RAFT Polymerisation"],"dc:type":["doctoral thesis","http://purl.org/coar/resource_type/c_db06"]},"updated_at":"2026-07-24T05:32:27Z"}