Molecular Dynamics Simulations Reveal a Dielectric-Responsive Coronal Structure in Protein鈥揚olymer Surfactant Hybrid Nanoconstructs
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- 作者：Alex P. S. Brogan ; Richard B. Sessions ; Adam W. Perriman ; Stephen Mann
- 刊名：Journal of the American Chemical Society
- 出版年：2014
- 出版时间：December 3, 2014
- 年：2014
- 卷：136
- 期：48
- 页码：16824-16831
- 全文大小：645K
- ISSN：1520-5126
文摘
Solvent-free liquid proteins are a new class of thermally stable hybrid bionanomaterials that are produced by extensive lyophilization of aqueous solutions of protein鈥損olymer surfactant nanoconjugates followed by thermal annealing. The hybrid constructs, which consist of a globular protein core surrounded by a monolayer of electrostatically coupled polymer surfactant molecules, exhibit nativelike structure, function, and backbone dynamics over a large temperature range. Despite the key importance of the polymer surfactant shell, very little is known about the atomistic structure of the corona and how it influences the phase behavior and properties of these novel nanoscale objects. Here we present molecular dynamics simulations of protein鈥損olymer surfactant nanoconjugates consisting of globular cores of myoglobin or lysozyme and demonstrate that the derived structural parameters are highly consistent with experimental values. We show that the coronal layer structure is responsive to the dielectric constant of the medium and that the mobility of the polymer surfactant molecules is significantly hindered in the solvent-free state, providing a basis for the origins of retained protein dynamics in these novel biofluids. Taken together, our results suggest that the extension of molecular dynamics simulations to hybrid nanoscale objects could be of generic value in diverse areas of soft matter chemistry, bioinspired engineering, and biomolecular nanotechnology.