Well‐Defined Poly(HPMAm) Brushes via Surface‐Initiated RAFT Polymerization; A Mixed‐Chain Transfer Agent (CTA) Approach

Abstract Over three decades, efforts to prevent non‐specific protein adsorption on surfaces have improved; however, developing well‐defined antifouling coatings remains a challenge in biomaterials research. In this study, a rapid and straightforward protocol relying on surface‐initiated reversible a...

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Main Authors: Manisha Singh, Zdeňka Sedláková, Jan Svoboda, Eliezer Jäger, Rafal Poreba
Format: Article
Language:English
Published: Wiley-VCH 2025-07-01
Series:Advanced Materials Interfaces
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Online Access:https://doi.org/10.1002/admi.202500196
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author Manisha Singh
Zdeňka Sedláková
Jan Svoboda
Eliezer Jäger
Rafal Poreba
author_facet Manisha Singh
Zdeňka Sedláková
Jan Svoboda
Eliezer Jäger
Rafal Poreba
author_sort Manisha Singh
collection DOAJ
description Abstract Over three decades, efforts to prevent non‐specific protein adsorption on surfaces have improved; however, developing well‐defined antifouling coatings remains a challenge in biomaterials research. In this study, a rapid and straightforward protocol relying on surface‐initiated reversible addition‐fragmentation chain‐transfer (RAFT) polymerization (S‐RAFT) is demonstrated to fabricate poly(N‐(2‐hydroxypropyl methacrylamide), poly(HPMAm)) brushes employing a mixed‐chain transfer agent (CTA) approach. By systematically evaluating different combinations of surface‐tethered and free CTAs, it is demonstrated that the simultaneous use of structurally distinct CTA classes; dithiobenzoate (DTB) and trithiocarbonate (TTC); enhances polymerization control and brush growth rates. The conditions enable the fabrication of poly(HPMAm) brushes exceeding 70 nm in thickness within only 4 h at 50 °C. Spectroscopic ellipsometry confirmed that the mixed‐CTA approach significantly outperforms single‐CTA systems, yielding higher polymerization efficiency and greater brush thickness. Additionally, size exclusion chromatography (SEC) confirmed that the solution‐born polymers exhibited narrow dispersity (Р= 1.05–1.15), ensuring well‐defined polymer structures. The findings highlight the advantages of combining different CTAs in a single polymerization system, leading to a more efficient and scalable method for fabricating antifouling poly(HPMAm) coatings. This approach offers a significant potential for biomedical applications, including biosensors, blood‐contacting devices, and implantable materials.
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spelling doaj-art-b60a9e370c0d4e959a52f8529bebda332025-08-20T03:12:49ZengWiley-VCHAdvanced Materials Interfaces2196-73502025-07-011213n/an/a10.1002/admi.202500196Well‐Defined Poly(HPMAm) Brushes via Surface‐Initiated RAFT Polymerization; A Mixed‐Chain Transfer Agent (CTA) ApproachManisha Singh0Zdeňka Sedláková1Jan Svoboda2Eliezer Jäger3Rafal Poreba4Institute of Macromolecular Chemistry Czech Academy of Sciences Heyrovsky sq. 2 Prague 16200 Czech RepublicInstitute of Macromolecular Chemistry Czech Academy of Sciences Heyrovsky sq. 2 Prague 16200 Czech RepublicInstitute of Macromolecular Chemistry Czech Academy of Sciences Heyrovsky sq. 2 Prague 16200 Czech RepublicInstitute of Macromolecular Chemistry Czech Academy of Sciences Heyrovsky sq. 2 Prague 16200 Czech RepublicInstitute of Macromolecular Chemistry Czech Academy of Sciences Heyrovsky sq. 2 Prague 16200 Czech RepublicAbstract Over three decades, efforts to prevent non‐specific protein adsorption on surfaces have improved; however, developing well‐defined antifouling coatings remains a challenge in biomaterials research. In this study, a rapid and straightforward protocol relying on surface‐initiated reversible addition‐fragmentation chain‐transfer (RAFT) polymerization (S‐RAFT) is demonstrated to fabricate poly(N‐(2‐hydroxypropyl methacrylamide), poly(HPMAm)) brushes employing a mixed‐chain transfer agent (CTA) approach. By systematically evaluating different combinations of surface‐tethered and free CTAs, it is demonstrated that the simultaneous use of structurally distinct CTA classes; dithiobenzoate (DTB) and trithiocarbonate (TTC); enhances polymerization control and brush growth rates. The conditions enable the fabrication of poly(HPMAm) brushes exceeding 70 nm in thickness within only 4 h at 50 °C. Spectroscopic ellipsometry confirmed that the mixed‐CTA approach significantly outperforms single‐CTA systems, yielding higher polymerization efficiency and greater brush thickness. Additionally, size exclusion chromatography (SEC) confirmed that the solution‐born polymers exhibited narrow dispersity (Р= 1.05–1.15), ensuring well‐defined polymer structures. The findings highlight the advantages of combining different CTAs in a single polymerization system, leading to a more efficient and scalable method for fabricating antifouling poly(HPMAm) coatings. This approach offers a significant potential for biomedical applications, including biosensors, blood‐contacting devices, and implantable materials.https://doi.org/10.1002/admi.202500196(surface RAFTpoly(HPMA))poly(HPMAm)polymer brushessacrificial chain transfer agentsurface‐initiated polymerization
spellingShingle Manisha Singh
Zdeňka Sedláková
Jan Svoboda
Eliezer Jäger
Rafal Poreba
Well‐Defined Poly(HPMAm) Brushes via Surface‐Initiated RAFT Polymerization; A Mixed‐Chain Transfer Agent (CTA) Approach
Advanced Materials Interfaces
(surface RAFT
poly(HPMA))
poly(HPMAm)
polymer brushes
sacrificial chain transfer agent
surface‐initiated polymerization
title Well‐Defined Poly(HPMAm) Brushes via Surface‐Initiated RAFT Polymerization; A Mixed‐Chain Transfer Agent (CTA) Approach
title_full Well‐Defined Poly(HPMAm) Brushes via Surface‐Initiated RAFT Polymerization; A Mixed‐Chain Transfer Agent (CTA) Approach
title_fullStr Well‐Defined Poly(HPMAm) Brushes via Surface‐Initiated RAFT Polymerization; A Mixed‐Chain Transfer Agent (CTA) Approach
title_full_unstemmed Well‐Defined Poly(HPMAm) Brushes via Surface‐Initiated RAFT Polymerization; A Mixed‐Chain Transfer Agent (CTA) Approach
title_short Well‐Defined Poly(HPMAm) Brushes via Surface‐Initiated RAFT Polymerization; A Mixed‐Chain Transfer Agent (CTA) Approach
title_sort well defined poly hpmam brushes via surface initiated raft polymerization a mixed chain transfer agent cta approach
topic (surface RAFT
poly(HPMA))
poly(HPMAm)
polymer brushes
sacrificial chain transfer agent
surface‐initiated polymerization
url https://doi.org/10.1002/admi.202500196
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