Photons and photocatalysts as limiting reagents for PET-RAFT photopolymerization
[Display omitted] •Typical batch PET-RAFT was found to be limited by photocatalyst and light intensity.•A universal scaling law was developed describing various geometries and reaction conditions.•Polymerization through oxygen approaches required a critical catalyst loading loadings.•PET-RAFT is sub...
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| Published in | Chemical engineering journal (Lausanne, Switzerland : 1996) Vol. 456; p. 141007 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Elsevier B.V
15.01.2023
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| Online Access | Get full text |
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| Abstract | [Display omitted]
•Typical batch PET-RAFT was found to be limited by photocatalyst and light intensity.•A universal scaling law was developed describing various geometries and reaction conditions.•Polymerization through oxygen approaches required a critical catalyst loading loadings.•PET-RAFT is subject to less retardation than conventional RAFT.
The kinetics of photoinduced electron/energy transfer - reversible addition fragmentation chain transfer (PET-RAFT) polymerization were investigated using a model system of methyl acrylate (MA) in the presence of trithiocarbonate chain transfer agents and tris(2-phenylpyridine)iridium(III) (Ir(ppy)3) as the photocatalyst. A powerful polymerization through oxygen approach was developed. Efficient PET-RAFT occurred under blue, violet, and green light with catalyst loadings of 10 ppm. Minimal polymerization was observed under orange or red light. Kinetic scaling analysis was developed to evaluate the impact of light intensity, catalyst loading and geometry of both the light source and the reaction vessel. A universal scaling law was developed for Ir(ppy)3 and other energy transfer catalyzed PET-RAFT, allowing both polymerization through oxygen and deoxygenated systems from the literature to be described across a range of light intensities, reaction conditions and geometries. Finally, the scaling analysis indicates that PET-RAFT systems should be subject to less retardation than conventional RAFT systems, due to the chain transfer agent being involved in radical generation steps. |
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| AbstractList | [Display omitted]
•Typical batch PET-RAFT was found to be limited by photocatalyst and light intensity.•A universal scaling law was developed describing various geometries and reaction conditions.•Polymerization through oxygen approaches required a critical catalyst loading loadings.•PET-RAFT is subject to less retardation than conventional RAFT.
The kinetics of photoinduced electron/energy transfer - reversible addition fragmentation chain transfer (PET-RAFT) polymerization were investigated using a model system of methyl acrylate (MA) in the presence of trithiocarbonate chain transfer agents and tris(2-phenylpyridine)iridium(III) (Ir(ppy)3) as the photocatalyst. A powerful polymerization through oxygen approach was developed. Efficient PET-RAFT occurred under blue, violet, and green light with catalyst loadings of 10 ppm. Minimal polymerization was observed under orange or red light. Kinetic scaling analysis was developed to evaluate the impact of light intensity, catalyst loading and geometry of both the light source and the reaction vessel. A universal scaling law was developed for Ir(ppy)3 and other energy transfer catalyzed PET-RAFT, allowing both polymerization through oxygen and deoxygenated systems from the literature to be described across a range of light intensities, reaction conditions and geometries. Finally, the scaling analysis indicates that PET-RAFT systems should be subject to less retardation than conventional RAFT systems, due to the chain transfer agent being involved in radical generation steps. |
| ArticleNumber | 141007 |
| Author | Nwoko, Tochukwu De Alwis Watuthanthrige, Nethmi Yehl, Kevin Parnitzke, Bryan Boyer, Cyrille Bradford, Kate G.E. Konkolewicz, Dominik |
| Author_xml | – sequence: 1 givenname: Bryan orcidid: 0000-0002-5049-2416 surname: Parnitzke fullname: Parnitzke, Bryan organization: Department of Chemistry and Biochemistry, Miami University, 651 E High St. Oxford, OH 45056, USA – sequence: 2 givenname: Tochukwu surname: Nwoko fullname: Nwoko, Tochukwu organization: Department of Chemistry and Biochemistry, Miami University, 651 E High St. Oxford, OH 45056, USA – sequence: 3 givenname: Kate G.E. surname: Bradford fullname: Bradford, Kate G.E. organization: Department of Chemistry and Biochemistry, Miami University, 651 E High St. Oxford, OH 45056, USA – sequence: 4 givenname: Nethmi surname: De Alwis Watuthanthrige fullname: De Alwis Watuthanthrige, Nethmi organization: Department of Chemistry and Biochemistry, Miami University, 651 E High St. Oxford, OH 45056, USA – sequence: 5 givenname: Kevin surname: Yehl fullname: Yehl, Kevin organization: Department of Chemistry and Biochemistry, Miami University, 651 E High St. Oxford, OH 45056, USA – sequence: 6 givenname: Cyrille surname: Boyer fullname: Boyer, Cyrille organization: Centre for Advanced Macromolecular Design, School of Chemical Engineering, The University of New South Wales, UNSW Sydney NSW 2052, Australia – sequence: 7 givenname: Dominik orcidid: 0000-0002-3828-5481 surname: Konkolewicz fullname: Konkolewicz, Dominik email: d.konkolewicz@miamiOH.edu organization: Department of Chemistry and Biochemistry, Miami University, 651 E High St. Oxford, OH 45056, USA |
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