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Hypothesis Polyzwitterions as a promising class of materials are often used to construct antifouling surfaces with optimized conformation and compositions for a wide variety of antifouling applications. While numerous zwitterionic polymers have been identified for their antifouling capacity, the exact relationship among molecular structure, surface hydration property, and antifouling performance of zwitterionic polymers at different scales still remains elusive. Experiments we first designed and synthesized a new zwitterionic monomer of 3-(4-(methacryloyloxy)-1-methylpiperidin-1-ium-1-yl)-propane-1-sulfonate (MAMPS), then used MAMPS monomers to fabricate into homogenous polymer brushes on Au substrate using SI-ATRP and heterogeneous double-network (DN) hydrogels combining with Agar network via one-pot, heating-cooling-photopolymerization method, and finally evaluated their antifouling ability to resist the adsorption of protein/cell/bacteria on the two different polymer forms at microscopic and macroscopic scales. Findings For microscopic polyMAMPS brushes, they exhibited excellent resistance to nonspecific protein adsorption from both undiluted blood serum/plasma (0.3–5 ng/cm2), cell adhesion up to 3 days, and clinically relevant bacterial attachment for 72 h at the optimal film thicknesses of 20–40 nm. For macroscopic Agar/polyMAMPS DN hydrogels, they also exhibited approximately 96% less protein adhesion than tissue culture polystyrene (TCPS). Different structured materials consisting of polyMAMPS at both micro- and macro-scales demonstrate its excellent, intrinsic antifouling property, which could be related to their highly water binding character of zwitterionic groups. PolyMAMPS materials, alternative to commonly used poly(sulfobetaine methacrylate) (polySBMA) and poly(carboxybetaine methacrylate) (polyCBMA) zwitterions, hold great promise for antifouling designs and applications.

Skin wound healing is a still long-history challenging problem and impeded by the foreign-body reaction including severe inflammation response, poor neovascularization, incomplete re-epithelialization and defective ECM remodeling. Development of biocompatible polymers, in combination with specific drugs or growth factors, has been considered as a promising strategy to treat skin wounds. Significant research efforts have been made to develop poly(ethylene glycol) PEG-based polymers for wound healing, however less efforts has been paid to zwitterionic materials, some of which have demonstrated their super low-fouling property in vitro and anti-inflammatory property in vivo. Here, we synthesized ultra-low-fouling zwitterionic sulfated poly(sulfobetaine methacrylate) (polySBMA) hydrogels and applied them to full-thickness cutaneous wounds in mice. The healing effects of SBMA hydrogels on the wound closure, re-epithelialization ratio, ECM remodeling, angiogenesis, and macrophage responses during wound healing processes were histologically evaluated by in vivo experiments. Collective results indicate that SBMA hydrogels promote full-thickness excisional acute wound regeneration in mice by enhancing angiogenesis, decreasing inflammation response, and modulating macrophage polarization. Consistently, the incorporation of SBMA into PEG hydrogels also improved the overall wound healing efficiency as compared to pure PEG hydrogels. This work demonstrates zwitterionic SBMA hydrogels as promising wound dressings for treating full-thickness excisional skin wounds. Statement of Significance Development of highly effective wound regeneration system is practically important for biomedical applications. Here, we synthesized ultra-low-fouling zwitterionic sulfated poly(sulfobetaine methacrylate) (polySBMA) hydrogels and applied it to full-thickness cutaneous wounds in mice, in comparison with PEG hydrogels as a control. We are the first to examine and reveal the difference between zwitterionic SBMA hydrogels and PEG hydrogels using a full-thickness excisional mice model. Overall, a series of in vivo systematic tests demonstrated that zwitterionic SBMA hydrogels exhibited superior wound healing property in almost all aspects as compared to PEG hydrogels.

Polymer brushes have been demonstrated as versatile and effective surface modification method to achieve unparalleled control over surface properties and functionality. Here, this review mainly highlights the intriguing performance and functionalities of zwitterionic polymer brushes with anti-polyelectrolyte property for a variety of applications in protein resistance, antibacterial activity, surface wetting, and surface frication. Different from other hydrophilic polymer brushes, zwitterionic brushes exhibit the unique zwitterionic-induced anti-polyelectrolyte effect, allowing for the development of new smart polymers and polymer-coated surfaces.