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Towards natural care products : Structural and deposition studies of bio-based polymer and surfactant mixtures

Del Giudice, Alessandra LU orcid ; Gubitosi, Marta LU ; Sthoer, Adrien ; Köhler, Sebastian LU ; Ayscough, Sophie LU ; Skoda, Maximilian W.A. ; Nylander, Tommy LU and Halthur, Tobias (2024) In Colloids and Surfaces A: Physicochemical and Engineering Aspects 698.
Abstract

Oppositely charged polymer-surfactant systems are expected to interact with formation of coacervate complexes near composition of charge-neutrality. Such behaviour is widely used in formulated products (e.g. household and personal care), where the co-deposition of coacervates and active ingredients on various surfaces is triggered by dilution. A transition towards the use of more sustainable ingredients is currently ongoing as a response to the need of more environmentally conscious choices in production, albeit slowed down by the often more complex and not fully understood bulk and interfacial behaviour of new ingredients. In this work, mixtures of a medium-chain fatty acid (sodium decanoate) and two grades of bio-based cationic... (More)

Oppositely charged polymer-surfactant systems are expected to interact with formation of coacervate complexes near composition of charge-neutrality. Such behaviour is widely used in formulated products (e.g. household and personal care), where the co-deposition of coacervates and active ingredients on various surfaces is triggered by dilution. A transition towards the use of more sustainable ingredients is currently ongoing as a response to the need of more environmentally conscious choices in production, albeit slowed down by the often more complex and not fully understood bulk and interfacial behaviour of new ingredients. In this work, mixtures of a medium-chain fatty acid (sodium decanoate) and two grades of bio-based cationic modified inulin were studied. The phase behaviour was determined in a wide composition matrix. The formation of coacervate complexes was observed for the mixture with the higher charge density polymer at a surfactant concentration of 1–3 wt%, close to the surfactant critical micellar concentration in pure water. Such behaviour was confirmed by DLS and SAXS data, suggesting surfactant-polymer complexation in a concentrated phase of packed micelles with a micelle-to-micelle distance of ∼4.5 nm. In situ ellipsometry and neutron reflectometry experiments were conducted to study the effect on surface deposition when diluting. The ellipsometry showed an adsorbed mass of ∼1.3–1.9 mg/m2, consistent with the deposition of a coacervate layer, and considerably higher than the neat, adsorbed polymer layer of ∼0.3 mg/m2. In the case of the neutron reflectometry experiments, dilution was performed before contact with the surface (pre-mixing), and no adsorption of coacervates was observed, but rather the adsorption of a polymer layer (0.49–0.85 mg/m2). The different results obtained with the different techniques highlight the kinetic nature of bulk coacervate formation and deposition, and the competition between these two phenomena. Maximal deposition can be achieved if one can control this time window either by tuning the composition of the system or the experimental set-up, to mimic the conditions of a specific application.

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author
; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Biopolymers, Bulk characterisation, Coacervates, Deposition, Fatty acids, Surfactants
in
Colloids and Surfaces A: Physicochemical and Engineering Aspects
volume
698
article number
134365
publisher
Elsevier
external identifiers
  • scopus:85196283623
ISSN
0927-7757
DOI
10.1016/j.colsurfa.2024.134365
language
English
LU publication?
yes
id
90ae5cab-bc1f-46cf-a8ac-be8d52a32e59
date added to LUP
2024-07-01 13:36:24
date last changed
2024-07-01 13:37:08
@article{90ae5cab-bc1f-46cf-a8ac-be8d52a32e59,
  abstract     = {{<p>Oppositely charged polymer-surfactant systems are expected to interact with formation of coacervate complexes near composition of charge-neutrality. Such behaviour is widely used in formulated products (e.g. household and personal care), where the co-deposition of coacervates and active ingredients on various surfaces is triggered by dilution. A transition towards the use of more sustainable ingredients is currently ongoing as a response to the need of more environmentally conscious choices in production, albeit slowed down by the often more complex and not fully understood bulk and interfacial behaviour of new ingredients. In this work, mixtures of a medium-chain fatty acid (sodium decanoate) and two grades of bio-based cationic modified inulin were studied. The phase behaviour was determined in a wide composition matrix. The formation of coacervate complexes was observed for the mixture with the higher charge density polymer at a surfactant concentration of 1–3 wt%, close to the surfactant critical micellar concentration in pure water. Such behaviour was confirmed by DLS and SAXS data, suggesting surfactant-polymer complexation in a concentrated phase of packed micelles with a micelle-to-micelle distance of ∼4.5 nm. In situ ellipsometry and neutron reflectometry experiments were conducted to study the effect on surface deposition when diluting. The ellipsometry showed an adsorbed mass of ∼1.3–1.9 mg/m<sup>2</sup>, consistent with the deposition of a coacervate layer, and considerably higher than the neat, adsorbed polymer layer of ∼0.3 mg/m<sup>2</sup>. In the case of the neutron reflectometry experiments, dilution was performed before contact with the surface (pre-mixing), and no adsorption of coacervates was observed, but rather the adsorption of a polymer layer (0.49–0.85 mg/m<sup>2</sup>). The different results obtained with the different techniques highlight the kinetic nature of bulk coacervate formation and deposition, and the competition between these two phenomena. Maximal deposition can be achieved if one can control this time window either by tuning the composition of the system or the experimental set-up, to mimic the conditions of a specific application.</p>}},
  author       = {{Del Giudice, Alessandra and Gubitosi, Marta and Sthoer, Adrien and Köhler, Sebastian and Ayscough, Sophie and Skoda, Maximilian W.A. and Nylander, Tommy and Halthur, Tobias}},
  issn         = {{0927-7757}},
  keywords     = {{Biopolymers; Bulk characterisation; Coacervates; Deposition; Fatty acids; Surfactants}},
  language     = {{eng}},
  publisher    = {{Elsevier}},
  series       = {{Colloids and Surfaces A: Physicochemical and Engineering Aspects}},
  title        = {{Towards natural care products : Structural and deposition studies of bio-based polymer and surfactant mixtures}},
  url          = {{http://dx.doi.org/10.1016/j.colsurfa.2024.134365}},
  doi          = {{10.1016/j.colsurfa.2024.134365}},
  volume       = {{698}},
  year         = {{2024}},
}