Branched Copolymer Surfactants as Versatile Templates for Responsive Emulsifiers with Bespoke Temperature‐Triggered Emulsion‐Breaking or Gelation

Abhishek Rajbanshi; Marcelo Alves da silva; Niamh Haslett; Philippa Cranwell; Neil Cunningham; Najet Mahmoudi; Darragh Murnane; Ewa Pavlova; Miroslav Slouf; Cecile Dreiss; Michael Cook

doi:10.1002/admi.202300755

Branched Copolymer Surfactants as Versatile Templates for Responsive Emulsifiers with Bespoke Temperature‐Triggered Emulsion‐Breaking or Gelation

Abhishek Rajbanshi, Marcelo Alves da silva, Niamh Haslett, Philippa Cranwell, Neil Cunningham, Najet Mahmoudi, Darragh Murnane, Ewa Pavlova, Miroslav Slouf, Cecile Dreiss, Michael Cook

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Abstract

It has been found that the thermoresponsive behavior of emulsions stabilized by block copolymer surfactants (BCSs) can induce either gelation or emulsion break-up with mild temperature changes. A hydrophilic, steric-stabilizing component of the BCS, polyethylene glycol methacrylate (PEGMA), is crucial to control the thermoresponsive behavior of the emulsions: longer PEG chains (950 g mol−1) lead to thermoregulation, whereas shorter PEGM chains (500 or 300 g mol−1) lead to emulsion break-up upon mild heating. Additionally, the relative abundance of PEGMA to the thermoresponsive component in the BCS controls the gelation temperature of BCS-stabilized emulsions. Small-angle neutron scattering and transmission electron microscopy reveal that the BCS forms oblate ellipsoids which grow anisotropically with temperature. In samples that form a gel, there is evidence that these nano-objects form supra-colloidal structures, which are responsible for the gel mesophase formation. An optimal BCS can form emulsions that transition from a liquid to gel state when warmed above 32 °C. This makes the system ideal for in situ gelation upon contact with the body. Overall, this study highlights the great potential of BCSs in generating thermoresponsive emulsions for drug delivery and other healthcare applications.

Original language	English
Article number	2300755
Journal	advanced materials interfaces
Volume	11
Issue number	1
Early online date	27 Oct 2023
DOIs	https://doi.org/10.1002/admi.202300755
Publication status	Published - 4 Jan 2024

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Branched Copolymer Surfactants_RAJBANSHI_Publishedonline27October2023_GOLD VoR (CC BY)Final published version, 4.25 MBLicence: CC BY

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Rajbanshi, A., Alves da silva, M., Haslett, N., Cranwell, P., Cunningham, N., Mahmoudi, N., Murnane, D., Pavlova, E., Slouf, M., Dreiss, C., & Cook, M. (2024). Branched Copolymer Surfactants as Versatile Templates for Responsive Emulsifiers with Bespoke Temperature‐Triggered Emulsion‐Breaking or Gelation. advanced materials interfaces, 11(1), Article 2300755. https://doi.org/10.1002/admi.202300755

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title = "Branched Copolymer Surfactants as Versatile Templates for Responsive Emulsifiers with Bespoke Temperature‐Triggered Emulsion‐Breaking or Gelation",

abstract = "It has been found that the thermoresponsive behavior of emulsions stabilized by block copolymer surfactants (BCSs) can induce either gelation or emulsion break-up with mild temperature changes. A hydrophilic, steric-stabilizing component of the BCS, polyethylene glycol methacrylate (PEGMA), is crucial to control the thermoresponsive behavior of the emulsions: longer PEG chains (950 g mol−1) lead to thermoregulation, whereas shorter PEGM chains (500 or 300 g mol−1) lead to emulsion break-up upon mild heating. Additionally, the relative abundance of PEGMA to the thermoresponsive component in the BCS controls the gelation temperature of BCS-stabilized emulsions. Small-angle neutron scattering and transmission electron microscopy reveal that the BCS forms oblate ellipsoids which grow anisotropically with temperature. In samples that form a gel, there is evidence that these nano-objects form supra-colloidal structures, which are responsible for the gel mesophase formation. An optimal BCS can form emulsions that transition from a liquid to gel state when warmed above 32 °C. This makes the system ideal for in situ gelation upon contact with the body. Overall, this study highlights the great potential of BCSs in generating thermoresponsive emulsions for drug delivery and other healthcare applications.",

author = "Abhishek Rajbanshi and {Alves da silva}, Marcelo and Niamh Haslett and Philippa Cranwell and Neil Cunningham and Najet Mahmoudi and Darragh Murnane and Ewa Pavlova and Miroslav Slouf and Cecile Dreiss and Michael Cook",

note = "Funding Information: The EPSRC is thanked for funding the research (EP/T00813X/1). The grant is also supported by equipment funded by the Royal Society Research Grant (RF17‐9915). Dr Daniel Lester at the Warwick Polymer Characterisation RTP is thanked for gel‐permeation chromatography on the BCS samples. The authors gratefully acknowledge the Science and Technology Facilities Council (STFC) for access to neutron beamtime at ISIS, and for the provision of sample preparation facilities (experiment 2220037). Funding Information: The EPSRC is thanked for funding the research (EP/T00813X/1). The grant is also supported by equipment funded by the Royal Society Research Grant (RF17-9915). Dr Daniel Lester at the Warwick Polymer Characterisation RTP is thanked for gel-permeation chromatography on the BCS samples. The authors gratefully acknowledge the Science and Technology Facilities Council (STFC) for access to neutron beamtime at ISIS, and for the provision of sample preparation facilities (experiment 2220037). Publisher Copyright: {\textcopyright} 2023 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH.",

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Rajbanshi, A, Alves da silva, M, Haslett, N, Cranwell, P, Cunningham, N, Mahmoudi, N, Murnane, D, Pavlova, E, Slouf, M, Dreiss, C & Cook, M 2024, 'Branched Copolymer Surfactants as Versatile Templates for Responsive Emulsifiers with Bespoke Temperature‐Triggered Emulsion‐Breaking or Gelation', advanced materials interfaces, vol. 11, no. 1, 2300755. https://doi.org/10.1002/admi.202300755

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T1 - Branched Copolymer Surfactants as Versatile Templates for Responsive Emulsifiers with Bespoke Temperature‐Triggered Emulsion‐Breaking or Gelation

AU - Rajbanshi, Abhishek

AU - Alves da silva, Marcelo

AU - Haslett, Niamh

AU - Cranwell, Philippa

AU - Cunningham, Neil

AU - Mahmoudi, Najet

AU - Murnane, Darragh

AU - Pavlova, Ewa

AU - Slouf, Miroslav

AU - Dreiss, Cecile

AU - Cook, Michael

N1 - Funding Information: The EPSRC is thanked for funding the research (EP/T00813X/1). The grant is also supported by equipment funded by the Royal Society Research Grant (RF17‐9915). Dr Daniel Lester at the Warwick Polymer Characterisation RTP is thanked for gel‐permeation chromatography on the BCS samples. The authors gratefully acknowledge the Science and Technology Facilities Council (STFC) for access to neutron beamtime at ISIS, and for the provision of sample preparation facilities (experiment 2220037). Funding Information: The EPSRC is thanked for funding the research (EP/T00813X/1). The grant is also supported by equipment funded by the Royal Society Research Grant (RF17-9915). Dr Daniel Lester at the Warwick Polymer Characterisation RTP is thanked for gel-permeation chromatography on the BCS samples. The authors gratefully acknowledge the Science and Technology Facilities Council (STFC) for access to neutron beamtime at ISIS, and for the provision of sample preparation facilities (experiment 2220037). Publisher Copyright: © 2023 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH.

PY - 2024/1/4

Y1 - 2024/1/4

N2 - It has been found that the thermoresponsive behavior of emulsions stabilized by block copolymer surfactants (BCSs) can induce either gelation or emulsion break-up with mild temperature changes. A hydrophilic, steric-stabilizing component of the BCS, polyethylene glycol methacrylate (PEGMA), is crucial to control the thermoresponsive behavior of the emulsions: longer PEG chains (950 g mol−1) lead to thermoregulation, whereas shorter PEGM chains (500 or 300 g mol−1) lead to emulsion break-up upon mild heating. Additionally, the relative abundance of PEGMA to the thermoresponsive component in the BCS controls the gelation temperature of BCS-stabilized emulsions. Small-angle neutron scattering and transmission electron microscopy reveal that the BCS forms oblate ellipsoids which grow anisotropically with temperature. In samples that form a gel, there is evidence that these nano-objects form supra-colloidal structures, which are responsible for the gel mesophase formation. An optimal BCS can form emulsions that transition from a liquid to gel state when warmed above 32 °C. This makes the system ideal for in situ gelation upon contact with the body. Overall, this study highlights the great potential of BCSs in generating thermoresponsive emulsions for drug delivery and other healthcare applications.

AB - It has been found that the thermoresponsive behavior of emulsions stabilized by block copolymer surfactants (BCSs) can induce either gelation or emulsion break-up with mild temperature changes. A hydrophilic, steric-stabilizing component of the BCS, polyethylene glycol methacrylate (PEGMA), is crucial to control the thermoresponsive behavior of the emulsions: longer PEG chains (950 g mol−1) lead to thermoregulation, whereas shorter PEGM chains (500 or 300 g mol−1) lead to emulsion break-up upon mild heating. Additionally, the relative abundance of PEGMA to the thermoresponsive component in the BCS controls the gelation temperature of BCS-stabilized emulsions. Small-angle neutron scattering and transmission electron microscopy reveal that the BCS forms oblate ellipsoids which grow anisotropically with temperature. In samples that form a gel, there is evidence that these nano-objects form supra-colloidal structures, which are responsible for the gel mesophase formation. An optimal BCS can form emulsions that transition from a liquid to gel state when warmed above 32 °C. This makes the system ideal for in situ gelation upon contact with the body. Overall, this study highlights the great potential of BCSs in generating thermoresponsive emulsions for drug delivery and other healthcare applications.

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DO - 10.1002/admi.202300755

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Branched Copolymer Surfactants as Versatile Templates for Responsive Emulsifiers with Bespoke Temperature‐Triggered Emulsion‐Breaking or Gelation

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