Concurrent control over sequence and dispersity in multiblock copolymers
Controlling monomer sequence and dispersity in synthetic macromolecules is a major goal in polymer science as both parameters determine materials’ properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable....
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| Published in: | Nature chemistry Vol. 14; no. 3; pp. 304 - 312 |
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| Main Authors: | , , , , , , |
| Format: | Journal Article |
| Language: | English |
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Nature Publishing Group UK
01.03.2022
Nature Publishing Group |
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| ISSN: | 1755-4330, 1755-4349, 1755-4349 |
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| Abstract | Controlling monomer sequence and dispersity in synthetic macromolecules is a major goal in polymer science as both parameters determine materials’ properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable. Here we report a simple, one pot and rapid synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining a high livingness, and good agreement between theoretical and experimental molecular weights and quantitative yields. Key to our approach is the regulation in the activity of the chain transfer agent during a controlled radical polymerization that enables the preparation of multiblocks with gradually ascending (
Ɖ
= 1.16 → 1.60), descending (
Ɖ
= 1.66 → 1.22), alternating low and high dispersity values (
Ɖ
= 1.17 → 1.61 → 1.24 → 1.70 → 1.26) or any combination thereof. We further demonstrate the potential of our methodology through the synthesis of highly ordered pentablock, octablock and decablock copolymers, which yield multiblocks with concurrent control over both sequence and dispersity.
Synthetic approaches that can simultaneously control both polymer sequence and dispersity are difficult to achieve. Now, a switchable RAFT agent that regulates chain transfer activity during controlled radical polymerization has been shown to enable the one-pot synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining high livingness. |
|---|---|
| AbstractList | Controlling monomer sequence and dispersity in synthetic macromolecules is a major goal in polymer science as both parameters determine materials’ properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable. Here we report a simple, one pot and rapid synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining a high livingness, and good agreement between theoretical and experimental molecular weights and quantitative yields. Key to our approach is the regulation in the activity of the chain transfer agent during a controlled radical polymerization that enables the preparation of multiblocks with gradually ascending (Ɖ = 1.16 → 1.60), descending (Ɖ = 1.66 → 1.22), alternating low and high dispersity values (Ɖ = 1.17 → 1.61 → 1.24 → 1.70 → 1.26) or any combination thereof. We further demonstrate the potential of our methodology through the synthesis of highly ordered pentablock, octablock and decablock copolymers, which yield multiblocks with concurrent control over both sequence and dispersity.Synthetic approaches that can simultaneously control both polymer sequence and dispersity are difficult to achieve. Now, a switchable RAFT agent that regulates chain transfer activity during controlled radical polymerization has been shown to enable the one-pot synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining high livingness. Controlling monomer sequence and dispersity in synthetic macromolecules is a major goal in polymer science as both parameters determine materials’ properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable. Here we report a simple, one pot and rapid synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining a high livingness, and good agreement between theoretical and experimental molecular weights and quantitative yields. Key to our approach is the regulation in the activity of the chain transfer agent during a controlled radical polymerization that enables the preparation of multiblocks with gradually ascending ( Ɖ = 1.16 → 1.60), descending ( Ɖ = 1.66 → 1.22), alternating low and high dispersity values ( Ɖ = 1.17 → 1.61 → 1.24 → 1.70 → 1.26) or any combination thereof. We further demonstrate the potential of our methodology through the synthesis of highly ordered pentablock, octablock and decablock copolymers, which yield multiblocks with concurrent control over both sequence and dispersity. Synthetic approaches that can simultaneously control both polymer sequence and dispersity are difficult to achieve. Now, a switchable RAFT agent that regulates chain transfer activity during controlled radical polymerization has been shown to enable the one-pot synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining high livingness. Controlling monomer sequence and dispersity in synthetic macromolecules is a major goal in polymer science as both parameters determine materials' properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable. Here we report a simple, one pot and rapid synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining a high livingness, and good agreement between theoretical and experimental molecular weights and quantitative yields. Key to our approach is the regulation in the activity of the chain transfer agent during a controlled radical polymerization that enables the preparation of multiblocks with gradually ascending (Ɖ = 1.16 → 1.60), descending (Ɖ = 1.66 → 1.22), alternating low and high dispersity values (Ɖ = 1.17 → 1.61 → 1.24 → 1.70 → 1.26) or any combination thereof. We further demonstrate the potential of our methodology through the synthesis of highly ordered pentablock, octablock and decablock copolymers, which yield multiblocks with concurrent control over both sequence and dispersity. Controlling monomer sequence and dispersity in synthetic macromolecules is a major goal in polymer science as both parameters determine materials' properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable. Here we report a simple, one pot and rapid synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining a high livingness, and good agreement between theoretical and experimental molecular weights and quantitative yields. Key to our approach is the regulation in the activity of the chain transfer agent during a controlled radical polymerization that enables the preparation of multiblocks with gradually ascending (Ɖ = 1.16 → 1.60), descending (Ɖ = 1.66 → 1.22), alternating low and high dispersity values (Ɖ = 1.17 → 1.61 → 1.24 → 1.70 → 1.26) or any combination thereof. We further demonstrate the potential of our methodology through the synthesis of highly ordered pentablock, octablock and decablock copolymers, which yield multiblocks with concurrent control over both sequence and dispersity.Controlling monomer sequence and dispersity in synthetic macromolecules is a major goal in polymer science as both parameters determine materials' properties and functions. However, synthetic approaches that can simultaneously control both sequence and dispersity remain experimentally unattainable. Here we report a simple, one pot and rapid synthesis of sequence-controlled multiblocks with on-demand control over dispersity while maintaining a high livingness, and good agreement between theoretical and experimental molecular weights and quantitative yields. Key to our approach is the regulation in the activity of the chain transfer agent during a controlled radical polymerization that enables the preparation of multiblocks with gradually ascending (Ɖ = 1.16 → 1.60), descending (Ɖ = 1.66 → 1.22), alternating low and high dispersity values (Ɖ = 1.17 → 1.61 → 1.24 → 1.70 → 1.26) or any combination thereof. We further demonstrate the potential of our methodology through the synthesis of highly ordered pentablock, octablock and decablock copolymers, which yield multiblocks with concurrent control over both sequence and dispersity. |
| Author | Truong, Nghia P. Wyers, Dries Anastasaki, Athina Junkers, Tanja Whitfield, Richard Harrisson, Simon Antonopoulou, Maria-Nefeli |
| Author_xml | – sequence: 1 givenname: Maria-Nefeli surname: Antonopoulou fullname: Antonopoulou, Maria-Nefeli organization: Laboratory of Polymeric Materials, Department of Materials, ETH Zürich – sequence: 2 givenname: Richard orcidid: 0000-0003-4787-2060 surname: Whitfield fullname: Whitfield, Richard organization: Laboratory of Polymeric Materials, Department of Materials, ETH Zürich – sequence: 3 givenname: Nghia P. orcidid: 0000-0001-9900-2644 surname: Truong fullname: Truong, Nghia P. organization: Laboratory of Polymeric Materials, Department of Materials, ETH Zürich, Monash Institute of Pharmaceutical Sciences, Monash University – sequence: 4 givenname: Dries orcidid: 0000-0003-0841-9917 surname: Wyers fullname: Wyers, Dries organization: Polymer Reaction Design Group, School of Chemistry, Monash University – sequence: 5 givenname: Simon surname: Harrisson fullname: Harrisson, Simon organization: Laboratoire de Chimie des Polymères Organiques, University of Bordeaux/ENSCBP/CNRS UMR5629 – sequence: 6 givenname: Tanja orcidid: 0000-0002-6825-5777 surname: Junkers fullname: Junkers, Tanja organization: Polymer Reaction Design Group, School of Chemistry, Monash University – sequence: 7 givenname: Athina orcidid: 0000-0002-6615-1026 surname: Anastasaki fullname: Anastasaki, Athina email: athina.anastasaki@mat.ethz.ch organization: Laboratory of Polymeric Materials, Department of Materials, ETH Zürich |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/34845344$$D View this record in MEDLINE/PubMed https://hal.science/hal-03830134$$DView record in HAL |
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| SubjectTerms | 639/638/455 639/638/455/941 Analytical Chemistry Biochemistry Chain transfer Chemical Sciences Chemistry Chemistry and Materials Science Chemistry/Food Science Copolymers Dispersion Inorganic Chemistry Macromolecular Substances Macromolecules Molecular Weight Organic Chemistry Physical Chemistry Polymerization Polymers |
| Title | Concurrent control over sequence and dispersity in multiblock copolymers |
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