Antifouling Activity of Bottlebrush Network Hydrogels

Mitigating the attachment of microorganisms to polymer biomaterials is critical for preventing hospital-acquired infections. Two chemical strategies to mitigate fouling include fabricating fouling-resistant surfaces, which typically present hydrophilic polymers, such as polyethylene glycol (PEG), or creating fouling-release surfaces, which are generally hydrophobic featuring polydimethylsiloxane (PDMS). Despite the demonstrated promise of employing PEG or PDMS, amphiphilic PEG/PDMS copolymer materials remain understudied. Here, for the first time, we investigated if phase-separated amphiphilic copolymers confounded microbial adhesion. We used bottlebrush amphiphilic PEG/PDMS co-networks and homopolymer networks to study bacterial adhesion across a library of gels (ϕ_PEG = 0.00, 0.21, 0.40, 0.55, 0.80, and 1.00). Hydrated atomic force microscopy measurements revealed that most of the gels had low surface roughness, less than 5 nm, and an elastic modulus of ∼80 kPa. Interestingly, the surface roughness and elastic modulus of the ϕ_PEG = 0.40 gel were twice as high as those of the other gels due to the presence of crystalline domains, as confirmed using polarized optical microscopy on the hydrated gel. The interactions of these six well-characterized gels with bacteria were determined using <i>Escherichia coli</i> K12 MG1655 and <i>Staphylococcus aureus</i> SH1000. The attachment of both microbes decreased by at least 60% on all polymer gels versus the glass controls. <i>S. aureus</i> adhesion peaked on the ϕ_PEG = 0.40, likely due to its increased elastic modulus, consistent with previous literature demonstrating that modulus impacts microbial adhesion. These findings suggest that hydrophilic, hydrophobic, and amphiphilic biomaterials effectively resist the early attachment of Gram-negative and Gram-positive microorganisms, providing guidance for the design of next-generation antifouling surfaces.