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Hydrophilic Aldehyde-Functional Polymer Brushes: Synthesis, Characterization, and Potential Bioapplications.
Emma E Brotherton1, Edwin C Johnson1, Mark J Smallridge2
1Dainton Building, Department of Chemistry, The University of Sheffield, Brook Hill, Sheffield, South Yorkshire S3 7HF, U.K.
Macromolecules
|March 20, 2023
Summary
Surface-initiated activators regenerated by electron transfer atom transfer radical polymerization (ARGET ATRP) created hydrophilic polymer brushes. Post-polymerization oxidation yielded aldehyde-functional brushes, enabling histidine conjugation and controlled protein adsorption.
Area of Science:
- Polymer Chemistry
- Surface Science
- Biomaterials
Background:
- Surface-initiated activators regenerated by electron transfer atom transfer radical polymerization (ARGET ATRP) is a controlled polymerization technique.
- Functional polymer brushes on surfaces are crucial for various applications, including biosensing and drug delivery.
- Developing efficient methods for surface functionalization is essential for tailoring material properties.
Purpose of the Study:
- To synthesize and characterize hydrophilic polymer brushes using ARGET ATRP.
- To explore a post-polymerization modification strategy to introduce aldehyde functionalities.
- To functionalize aldehyde-terminated brushes with histidine and investigate protein adsorption behavior.
Main Methods:
- Surface-initiated ARGET ATRP of a cis-diol-functional methacrylic monomer (GEO5MA) from silicon wafers.
- Oxidation of the resulting polymer brushes using sodium periodate to create aldehyde functionalities.
- Functionalization with histidine via Schiff base chemistry and reductive amination, analyzed by XPS and ζ potential measurements.
- Protein adsorption studies using quartz crystal microbalance.
Main Results:
- Hydrophilic polymer brushes with thicknesses of 40-120 nm were successfully grown.
- Post-polymerization oxidation provided thicker aldehyde-functional brushes compared to direct polymerization of aldehyde monomers.
- Histidine conjugation achieved ~81% functionalization, uniformly distributed within the brush.
- Histidine-functionalized brushes exhibited pH-dependent zwitterionic behavior.
- Minimal protein adsorption on non-functionalized brushes, but strong adsorption on aldehyde-functionalized brushes.
Conclusions:
- Post-polymerization modification offers a superior route to aldehyde-functional polymer brushes.
- Histidine functionalization imparts tunable surface properties and controlled protein interactions.
- These functionalized brushes show promise for applications requiring specific biomolecular interactions and antifouling properties.
