Bactericidal and Hemocompatible Coating via the Mixed-Charged Copolymer.

Cationic antibacterial coating based on quaternary ammonium compounds, with an efficient and broad spectrum bactericidal property, has been widely used in various fields. However, the high density of positive charges tends to induce weak hemocompatibility, which hinders the application of the cationic antibacterial coating in blood-contacting devices and implants. It has been reported that a negatively charged surface can reduce blood coagulation, showing improved hemocompatibility. Here, we describe a strategy to combine the cationic and anionic groups by using mixed-charged copolymers. The copolymers of poly (quaternized vinyl pyridine- co- n-butyl methacrylate- co-methacrylate acid) [P(QVP- co- nBMA- co-MAA)] were synthesized through free radical copolymerization. The cationic group of QVP, the anionic group of MAA, and the hydrophobic group of nBMA were designed to provide bactericidal capability, hemocompatibility, and coating stability, respectively. Our findings show that the hydrophilicity of the copolymer coating increased, and its zeta potential decreased from positive charge to negative charge with the increase of the anionic/cationic ratio. Meanwhile, the bactericidal property of the copolymer coating was kept around a similar level compared with the pure quaternary ammonium copolymer coating. Furthermore, the coagulation time, platelet adhesion, and hemolysis tests revealed that the hemocompatibility of the copolymer coating improved with the addition of the anionic group. The mixed-charged copolymer combined both bactericidal property and hemocompatibility and has a promising potential in blood-contacting antibacterial devices and implants.

Mechanical Adaptability of the MMP-Responsive Film Improves the Functionality of Endothelial Cell Monolayer.

Extracellular matrix and cells are inherent in coordinating and adapting to each other during all physiological and pathological processes. Synthetic materials, however, show rarely reciprocal and spatiotemporal responses to cells, and lacking self-adapting properties as well. Here, a mechanical adaptability based on the matrix metalloproteinase (MMPs) sensitive polyelectrolyte film is reported. Poly-lysine (PLL) and methacrylated hyaluronic acid (HA-MA) nanolayers are employed to build the thin film through the layer-by-layer assembly, and it is further crosslinked using MMP sensitive peptides, which endows the films with changeable mechanical properties in response to MMPs. It is demonstrated that stiffness of the (PLL/HA-MA) films increases with the crosslinking, and then decreases in response to a treatment of enzyme. Consequently, the crosslinked (PLL/HA-MA) films reveal effective growth of endothelial cells (ECs), leading to fast formation of EC monolayer. Importantly, significantly improved endothelial function of the EC monolayer, which is characterized by integrity, biomolecules release, expression of function related gene, and antithrombotic properties, is achieved along with the decrosslinking of the film because of EC-secreted MMPs. These results suggest that mechanical adaptability of substrate in Young's modulus plays a significant role in endothelial progression, which shows great application potential in tissue engineering, regenerative medicine, and organ-on-a-chip.

Infusing Lubricant onto Erasable Microstructured Surfaces toward Guided Sliding of Liquid Droplets.

Introducing a lubricant layer onto surfaces has emerged as a novel strategy to address a wide range of interface-related challenges. Recent studies of lubricant-infused surfaces have extended beyond repelling liquids to manipulating the mobility of fluids. In this study, we report a design of slippery surfaces based on infusing lubricant onto a polyelectrolyte multilayer film whose surface microstructures can be erased rapidly under mild condition. Unlike other lubricant-infused surfaces, the liquid movements (e.g., moving resistance and direction) on such surfaces can be manipulated via programming the surface microstructures beforehand. The work reported here offers a versatile design concept of lubricant-infused surfaces and may turn on new applications of this emerging class of bioinspired materials.

Improved Endothelial Function of Endothelial Cell Monolayer on the Soft Polyelectrolyte Multilayer Film with Matrix-Bound Vascular Endothelial Growth Factor.

Endothelialization on the vascular implants is of great importance for prevention of undesired postimplantation symptoms. However, endothelial dysfunction of regenerated endothelial cell (EC) monolayer has been frequently observed, leading to severe complications, such as neointimal hyperplasia, late thrombosis, and neoatherosclerosis. It has significantly impeded long-term success of the therapy. So far, very little attention has been paid on endothelial function of EC monolayer. Bioinspired by the microenvironment of the endothelium in a blood vessel, this study described a soft polyelectrolyte multilayer film (PEM) through layer-by-layer assembly of poly(l-lysine) (PLL) and hyaluronan (HA). The (PLL/HA) PEM was chemically cross-linked and further incorporated with vascular endothelial growth factor. It demonstrated that this approach could promote EC adhesion and proliferation, further inducing formation of EC monolayer. Further, improved endothelial function of the EC monolayer was achieved as shown with the tighter integrity, higher production of nitric oxide, and expression level of endothelial function related genes, compared to EC monolayers on traditional substrates with high stiffness (e.g., glass, tissue culture polystyrene, and stainless steel). Our findings highlighted the influence of substrate stiffness on endothelial function of EC monolayer, giving a new strategy in the surface design of vascular implants.

Self-Healing Spongy Coating for Drug "Cocktail" Delivery.

Optimized ratio in the codelivery of therapeutics is of crucial importance to promote the synergism rather than the antagonistic effects. In this study, a self-healing spongy coating was described to facilitate the surface-mediated delivery of drug "cocktails" proportionally. The formation of spongy structures within the coating was achieved by acidic treatment and freeze-drying. Various drug combinations can be readily integrated through wicking method and subsequent micropore self-healing. The ratio of drug loading can be precisely regulated by the composition of loading solution and the embedded drugs were released in proportion according to the initial ratio of drug combination.

CuSO4/H2O2-Induced Rapid Deposition of Polydopamine Coatings with High Uniformity and Enhanced Stability.

Mussel-inspired polydopamine (PDA) deposition offers a promising route to fabricate multifunctional coatings for various materials. However, PDA deposition is generally a time-consuming process, and PDA coatings are unstable in acidic and alkaline media, as well as in polar organic solvents. We report a strategy to realize the rapid deposition of PDA by using CuSO4/H2O2 as a trigger. Compared to the conventional processes, our strategy shows the fastest deposition rate reported to date, and the PDA coatings exhibit high uniformity and enhanced stability. Furthermore, the PDA-coated porous membranes have excellent hydrophilicity, anti-oxidant properties, and antibacterial performance. This work demonstrates a useful method for the environmentally friendly, cost-effective, and time-saving fabrication of PDA coatings.

Dynamic spongy films to immobilize hydrophobic antimicrobial peptides for self-healing bactericidal coating.

A constant increase of nosocomial infections that are caused by adhesion and colonization of pathogenic microorganisms, especially drug-resistant bacteria, on the surfaces of healthcare devices has received considerable attention worldwide. In this study, bioinspired by antimicrobial skins of natural living beings, we developed a self-healing bactericidal coating through the immobilization of hydrophobic antimicrobial peptides (AMPs) into a multilayer film, which was constructed through the enhanced exponential layer-by-layer assembly of polyethylenimine (PEI) and poly(acrylic acid) (PAA). The (PEI/PAA) film shows particular dynamic properties from the as-prepared thin solid film to a spongy microporous structure via acid solution treatment, and then back to the thin solid film by eliminating micropores via the treatment of saturated humidity. Consequently, the loading and integration of hydrophobic AMPs such as gramicidin A (GA) into the (PEI/PAA) film were achieved via simple wicking action with GA solution and subsequent humidity treatment, respectively. The GA loading densities can be precisely controlled by using different concentrations of GA solution. We demonstrated that the GA immobilized (PEI/PAA) film has rapid self-healing properties, and that Gram-positive bacteria S. aureus including the methicillin-resistant type were efficiently killed through the contact-killing mode. Collectively, this self-healing bactericidal coating shows practical potential in a variety of healthcare applications.