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Zwitterionic materials are an important class of antifouling biomaterials for various applications. Despite such desirable antifouling properties, molecular-level understanding of the structure–property relationship associated with surface chemistry/topology/hydration and antifouling performance still remains to be elucidated. In this work, we computationally studied the packing structure, surface hydration, and antifouling property of three zwitterionic polymer brushes of poly(carboxybetaine methacrylate) (pCBMA), poly(sulfobetaine methacrylate) (pSBMA), and poly((2-(methacryloyloxy)ethyl)phosporylcoline) (pMPC) brushes and a hydrophilic PEG brush using a combination of molecular mechanics (MM), Monte Carlo (MC), molecular dynamics (MD), and steered MD (SMD) simulations. We for the first time determined the optimal packing structures of all polymer brushes from a wide variety of unit cells and chain orientations in a complex energy landscape. Under the optimal packing structures, MD simulations were further conducted to study the structure, dynamics, and orientation of water molecules and protein adsorption on the four polymer brushes, while SMD simulations to study the surface resistance of the polymer brushes to a protein. The collective results consistently revealed that the three zwitterionic brushes exhibited stronger interactions with water molecules and higher surface resistance to a protein than the PEG brush. It was concluded that both the carbon space length between zwitterionic groups and the nature of the anionic groups have a distinct effect on the antifouling performance, leading to the following antifouling ranking of pCBMA > pMPC > pSBMA. This work hopefully provides some structural insights into the design of new antifouling materials beyond traditional PEG-based antifouling materials.more » « less
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null (Ed.)Stimuli-responsive hydrogel strain sensors that synergize the advantages of both soft-wet hydrogels and smart functional materials have attracted rapidly increasing interest for exploring the opportunities from material design principles to emerging applications in electronic skins, health monitors, and human–machine interfaces. Stimuli-responsive hydrogel strain sensors possess smart and on-demand ability to specifically recognize various external stimuli and convert them into strain-induced mechanical, thermal, optical, and electrical signals. This review presents an up-to-date summary over the past five years on hydrogel strain sensors from different aspects, including material designs, gelation/fabrication methods, stimuli-responsive principles, and sensing performance. Hydrogel strain sensors are classified into five major categories based on the nature of the stimuli, and representative examples from each category are carefully selected and discussed in terms of structures, response mechanisms, and potential medical applications. Finally, current challenges and future perspectives of hydrogel strain sensors are tentatively proposed to stimulate more and better research in this emerging field.more » « less
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