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Interfacial Energy and Composition Controlled Self‐Stratification in Polyurethane Coatings.

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Title: Interfacial Energy and Composition Controlled Self‐Stratification in Polyurethane Coatings.
Authors: Singhal, Gaurav1 (AUTHOR), Lao, Lihong1 (AUTHOR), Pacholski, Michaeleen L.2 (AUTHOR), Shah, Harshad3 (AUTHOR), Gu, Junsi2 (AUTHOR), Caruso, Bryan2 (AUTHOR), Aguirre‐Vargas, Fabio3 (AUTHOR), Singh, Piyush1 (AUTHOR), Patankar, Kshitish A.2 (AUTHOR), Rogers, Simon A.4 (AUTHOR), Schroeder, Charles M.5 (AUTHOR), Braun, Paul V.5 (AUTHOR) pbraun@illinois.edu
Source: Macromolecular Materials & Engineering. Mar2026, Vol. 311 Issue 3, p1-12. 12p.
Subjects: Polyurethanes, Surface energy, Polymers, Coatings industry, Phase separation, Surface tension, Polymer blends, Polyols
Abstract: Self‐stratifying polymer systems are of great interest for coatings, as such systems reduce the time, cost, and environmental impact associated with the application of multilayered coatings by providing several layers in a single coating step. We have developed an understanding of self‐stratification in polyurethane systems that occurs when hydrophobic and hydrophilic polyols containing ethylene oxide, propylene oxide, and butylene oxide mers and prepolymers containing toluene diisocyanate and methylene diphenyl diisocyanate are mixed and cured. When these components are mixed in appropriate proportions, self‐stratification occurs where the hydrophobic component migrates to the air interface and the hydrophilic component to the substrate interface, with a thin hydrophobic layer present at the substrate walls when the substrate is hydrophobic. Self‐stratification requires less than 60 min, significantly less than the time required for the storage modulus to crossover the loss modulus (∼5 h). SIMS, XPS, and confocal Raman show that the stratification process at the air and substrate interfaces is dependent on interfacial surface energies, with the thickness and composition of the up to 10 µm thick interfacial region at the substrate controlled by the substrate surface energy. Self‐stratification is observed in both the bulk and thicknesses conventionally associated with coatings (10s of µm). [ABSTRACT FROM AUTHOR]
Copyright of Macromolecular Materials & Engineering is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Data: Interfacial Energy and Composition Controlled Self‐Stratification in Polyurethane Coatings.
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  Data: <searchLink fieldCode="AR" term="%22Singhal%2C+Gaurav%22">Singhal, Gaurav</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Lao%2C+Lihong%22">Lao, Lihong</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Pacholski%2C+Michaeleen+L%2E%22">Pacholski, Michaeleen L.</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Shah%2C+Harshad%22">Shah, Harshad</searchLink><relatesTo>3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Gu%2C+Junsi%22">Gu, Junsi</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Caruso%2C+Bryan%22">Caruso, Bryan</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Aguirre‐Vargas%2C+Fabio%22">Aguirre‐Vargas, Fabio</searchLink><relatesTo>3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Singh%2C+Piyush%22">Singh, Piyush</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Patankar%2C+Kshitish+A%2E%22">Patankar, Kshitish A.</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Rogers%2C+Simon+A%2E%22">Rogers, Simon A.</searchLink><relatesTo>4</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Schroeder%2C+Charles+M%2E%22">Schroeder, Charles M.</searchLink><relatesTo>5</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Braun%2C+Paul+V%2E%22">Braun, Paul V.</searchLink><relatesTo>5</relatesTo> (AUTHOR)<i> pbraun@illinois.edu</i>
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  Data: <searchLink fieldCode="JN" term="%22Macromolecular+Materials+%26+Engineering%22">Macromolecular Materials & Engineering</searchLink>. Mar2026, Vol. 311 Issue 3, p1-12. 12p.
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  Data: <searchLink fieldCode="DE" term="%22Polyurethanes%22">Polyurethanes</searchLink><br /><searchLink fieldCode="DE" term="%22Surface+energy%22">Surface energy</searchLink><br /><searchLink fieldCode="DE" term="%22Polymers%22">Polymers</searchLink><br /><searchLink fieldCode="DE" term="%22Coatings+industry%22">Coatings industry</searchLink><br /><searchLink fieldCode="DE" term="%22Phase+separation%22">Phase separation</searchLink><br /><searchLink fieldCode="DE" term="%22Surface+tension%22">Surface tension</searchLink><br /><searchLink fieldCode="DE" term="%22Polymer+blends%22">Polymer blends</searchLink><br /><searchLink fieldCode="DE" term="%22Polyols%22">Polyols</searchLink>
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  Label: Abstract
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  Data: Self‐stratifying polymer systems are of great interest for coatings, as such systems reduce the time, cost, and environmental impact associated with the application of multilayered coatings by providing several layers in a single coating step. We have developed an understanding of self‐stratification in polyurethane systems that occurs when hydrophobic and hydrophilic polyols containing ethylene oxide, propylene oxide, and butylene oxide mers and prepolymers containing toluene diisocyanate and methylene diphenyl diisocyanate are mixed and cured. When these components are mixed in appropriate proportions, self‐stratification occurs where the hydrophobic component migrates to the air interface and the hydrophilic component to the substrate interface, with a thin hydrophobic layer present at the substrate walls when the substrate is hydrophobic. Self‐stratification requires less than 60 min, significantly less than the time required for the storage modulus to crossover the loss modulus (∼5 h). SIMS, XPS, and confocal Raman show that the stratification process at the air and substrate interfaces is dependent on interfacial surface energies, with the thickness and composition of the up to 10 µm thick interfacial region at the substrate controlled by the substrate surface energy. Self‐stratification is observed in both the bulk and thicknesses conventionally associated with coatings (10s of µm). [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
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  Data: <i>Copyright of Macromolecular Materials & Engineering is the property of Wiley-Blackwell and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.1002/mame.202500424
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      – Code: eng
        Text: English
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        PageCount: 12
        StartPage: 1
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      – SubjectFull: Polyurethanes
        Type: general
      – SubjectFull: Surface energy
        Type: general
      – SubjectFull: Polymers
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      – SubjectFull: Coatings industry
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      – SubjectFull: Polymer blends
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              Text: Mar2026
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