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Porous surfaces have attracted tremendous interest for customized incorporation of functional agents on biomedical devices. However, the versatile preparation of porous structures on complicated devices remains challenging. Herein, we proposed a simple and robust method to fabricate "spongy skin" on diversified polymeric substrates based on non-solvent-induced phase separation (NIPS). Through the swelling and the subsequent phase separation process, interconnected porous structures were directly formed onto the polymeric substrates. The thickness and pore size could be regulated in the ranges of 5-200 and 0.3-0.75 μm, respectively. The fast capillary action of the porous structure enabled controllable loading and sustained release of ofloxacin and bovine albumin at a high loading dosage of 79.9 and 24.1 μg/cm 2 , respectively. We verified that this method was applicable to diversified materials including polymethyl methacrylate, polystyrene, thermoplastic polyurethane, polylactide acid, and poly(lactic- co -glycolic acid) and can be realized onto TCPS cell culture plates. This NIPS-based method is promising to generate porous surfaces on medical devices for incorporating therapeutic agents.

Developing surfaces that realize lubrication and durable wear resistance under high pressure has great implications in areas ranging from electromechanical systems to advanced biomedical devices but has proven challenging. Inspired by the zonal and transitional structure of articular cartilage, we fabricate a hydrogel-elastomer hybrid surface, where the hydrogel interpenetrates into the polymer elastomer substrate as a transitional and bonding zone, that exhibits a low coefficient of friction and wear resistance under a high load. First, we entrap benzophenone within the surface of polymer substrates such as polydimethylsiloxane, polyvinylchloride, and polyurethane. The hybrid surface is then achieved through initiating polymerization of the acrylamide monomer on the polymer surface upon ultraviolet irradiation. We observe an interpenetration area of the hydrogel and the polymer substrate. The hybrid surface shows a low coefficient of friction (∼0.05) under a very high load (over 100 atm contact pressure). It conserves the lubrication property over 100,000 cycles under a 10.9 MPa pressure and shows slight wear. This work brings a new perspective on designing surfaces with a lubrication property and wear resistance, showing broad applications.

Inspired by nature, many functional surfaces have been developed with special structures in biology, chemistry, and materials. Many research studies have been focused on the preparation of surfaces with static structure. Achieving dynamical manipulation of surface structure is desired but still a great challenge. Herein, a polyelectrolyte film capable of regional and reversible changes in the microporous structure is presented. Our proposal is based on the combination of azobenzene (Azo) π-π stacking and electrostatic interaction, which could be affected respectively by ultraviolet (UV) irradiation and water plasticization, to tune the mobility of polyelectrolyte chains. The porous patterns can be obtained after regional ultraviolet irradiation and acid treatment. Owing to the reversibility of Azo π-π stacking and electrostatic interaction, the patterns can be repeatedly created and erased in the polyelectrolyte film made by layer-by-layer (LbL) self-assembly of poly(ethyleneimine)-azo and poly(acrylic acid). Furthermore, through two rounds of porous pattern formation and erasure, different functional species can be loaded separately and confined regionally within the film, showing potential applications in the functional surface. This work highlights the coordination of two noncovalent interactions in thin films for regional and reversible controlling its structure, opening a window for more in-depth development of functional surfaces.

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.

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.

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.

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.

Infections associated with medical devices have become a major concern. The adhesion of bacteria to the devices' surfaces during the initial 24 h is believed to be a "decisive period" for implant-associated infections, which pose key challenges to optimal antiadhesion of microbes in this period. Herein, we have designed and constructed a (heparin/chitosan)10-(polyvinylpyrrolidone/poly(acrylic acid))10 [(HEP/CHI)10-(PVP/PAA)10] multilayer film by layer-by-layer self-assembly. Assembly of the underlying (HEP/CHI)10 multilayer film is based on electrostatic interactions, showing the properties of contact killing of bacteria. Deposition of the top (PVP/PAA)10 multilayer film is based on hydrogen bond interactions. The PAA molecules are then cross-linked to form anhydride groups by thermal treatment at 110 °C for 16 h. Therefore, it shows a top-down degradable capability in the determined period, leading to almost no adhesion of bacteria in 24 h. Our system combining the adhesion resistance and the contact killing properties shows an enhanced antibacterial capability through targeting the "decisive period" of implantation may have great potential for applications in medical implants, tissue engineering, etc.