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Engineering thermoresponsive emulsions with branched copolymer surfactants

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Marcelo A. Da Silva, Abhishek Rajbanshi, Daniel Achampong, Najet Mahmoudi, Lionel Porcar, Philipp Gutfreund, Andrea Tummino, Armando Maestro, Cecile A. Dreiss, Michael T. Cook

Original languageEnglish
Article number2200321
JournalMACROMOLECULAR MATERIALS AND ENGINEERING
Volume307
Issue number10
Early online date21 Aug 2022
DOIs
Accepted/In press8 Aug 2022
E-pub ahead of print21 Aug 2022
PublishedOct 2022

Bibliographical note

Funding Information: This work benefited from the use of the SasView application, originally developed under NSF award DMR‐0520547. SasView also contains code developed with funding from the European Union's Horizon 2020 Research and Innovation Programme under the SINE2020 project, grant agreement No 654000. Experiments at the ISIS Neutron and Muon Source were supported by a beamtime allocation RB2000184 for Sans2d from the Science and Technology Facilities Council (10.5286/ISIS.E.RB2000184). The authors thank Institut Laue Langevin for the provision of neutron beam time on D11 instrument (10.5291/ILL‐DATA.9‐11‐2028) and on Figaro instrument (10.5291/ILL‐DATA.9‐11‐2028). The Engineering and Physical Sciences Research Council (EP/T00813X/1) and Royal Society of Chemistry (RF17‐9915) are acknowledged for funding the research. The Royal Society of Chemistry and the Analytical Chemistry Trust Fund are also thanks for sponsoring the summer research project of D.O‐A. The authors would like to thank the reviewers of Macromolecular Materials and Engineering for their substantial contribution to improving the manuscript. Funding Information: This work benefited from the use of the SasView application, originally developed under NSF award DMR-0520547. SasView also contains code developed with funding from the European Union's Horizon 2020 Research and Innovation Programme under the SINE2020 project, grant agreement No 654000. Experiments at the ISIS Neutron and Muon Source were supported by a beamtime allocation RB2000184 for Sans2d from the Science and Technology Facilities Council (10.5286/ISIS.E.RB2000184). The authors thank Institut Laue Langevin for the provision of neutron beam time on D11 instrument (10.5291/ILL-DATA.9-11-2028) and on Figaro instrument (10.5291/ILL-DATA.9-11-2028). The Engineering and Physical Sciences Research Council (EP/T00813X/1) and Royal Society of Chemistry (RF17-9915) are acknowledged for funding the research. The Royal Society of Chemistry and the Analytical Chemistry Trust Fund are also thanked for sponsoring the summer research project of D.O-A. The authors would like to thank the reviewers of Macromolecular Materials and Engineering for their substantial contribution to improving the manuscript. Publisher Copyright: © 2022 The Authors. Macromolecular Materials and Engineering published by Wiley-VCH GmbH.

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Abstract

This study describes thermo-rheological properties of branched copolymer surfactants (BCSs) stabilizing oil-in-water emulsions to generate materials exhibiting temperature-dependent gelation with the ability to solubilize a broad range of molecules. Four poly(N-isopropylacrylamide-ran-poly(ethylene glycol) methacrylate) (poly(NIPAM-ran-PEGMA)) BCSs with varying molecular weight (Mn), 4.7; 7.0; 7.8 and 9.0 kg mol−1, are investigated via oscillatory shear rheology, small angle neutron scattering (SANS), and neutron reflectivity (NR). Rheological thermoscans show that emulsions stabilized by the BCS with the lowest Mn (4.7 kg mol−1) are thermo-thinning, while with the other BCSs the emulsions display a thermo-thickening behavior. Emulsions stabilized with the BCS with Mn = 7.8 kg mol−1 form gels within a precise temperature window depending on BCS concentration. Small angle neutron scattering data analysis suggests that the BCS is present in two forms in equilibrium, small aggregates dispersed in the bulk water and an adsorbed polymeric layer at the oil/water interface. Changes in dimensions of these structures with temperature correlate with the macroscopic thermo-thinning/thermo-thickening behavior observed. Neutron reflectivity is conducted at the oil/water interface to allow further elucidation of BCS behavior in these systems.

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