Biomolecular adsorption at aqueous silver interfaces : first-principles calculations, polarizable force-field simulations and comparisons with gold

Hughes, Zak E., Wright, Louise B. and Walsh, Tiffany R. 2013, Biomolecular adsorption at aqueous silver interfaces : first-principles calculations, polarizable force-field simulations and comparisons with gold, Langmuir, vol. 29, no. 43, pp. 13217-13229.

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Title Biomolecular adsorption at aqueous silver interfaces : first-principles calculations, polarizable force-field simulations and comparisons with gold
Author(s) Hughes, Zak E.
Wright, Louise B.
Walsh, Tiffany R.
Journal name Langmuir
Volume number 29
Issue number 43
Start page 13217
End page 13229
Total pages 13
Publisher American Chemical Society
Place of publication Washington, D.C.
Publication date 2013
ISSN 0743-7463
1520-5827
Summary The molecular simulation of biomolecules adsorbed at noble metal interfaces can assist in the development of bionanotechnology applications. In line with advances in polarizable force fields for adsorption at aqueous gold interfaces, there is scope for developing a similar force field for silver. One way to accomplish this is via the generation of in vacuo adsorption energies calculated using first-principles approaches for a wide range of different but biologically relevant small molecules, including water. Here, we present such first-principles data for a comprehensive range of bioorganic molecules obtained from plane-wave density functional theory calculations using the vdW-DF functional. As reported previously for the gold force field, GolP-CHARMM (Wright, L. B.; Rodger, P. M.; Corni, S.; Walsh, T. R. GolP-CHARMM: firstprinciples based force-fields for the interaction of proteins with Au(111) and Au(100). J. Chem. Theory Comput. 2013, 9, 1616− 1630), we have used these data to construct a a new force field, AgP-CHARMM, suitable for the simulation of biomolecules at the aqueous Ag(111) and Ag(100) interfaces. This force field is derived to be consistent with GolP-CHARMM such that adsorption on Ag and Au can be compared on an equal footing. Our force fields are used to evaluate the water overlayer stability on both silver and gold, finding good agreement with known behaviors. We also calculate and compare the structuring (spatial and orientational) of liquid water adsorbed at both silver and gold. Finally, we report the adsorption free energy of a range of amino acids at both the Au(111) and Ag(111) aqueous interfaces, calculated using metadynamics. Stronger adsorption on gold was noted in most cases, with the exception being the carboxylate group present in aspartic acid. Our findings also indicate differences in the binding free energy profile between silver and gold for some amino acids, notably for His and Arg. Our analysis suggests that the relatively stronger structuring of the first water layer on silver, relative to gold, could give rise to these differences.
Language eng
Field of Research 030603 Colloid and Surface Chemistry
030701 Quantum Chemistry
030704 Statistical Mechanics in Chemistry
Socio Economic Objective 970103 Expanding Knowledge in the Chemical Sciences
HERDC Research category C1 Refereed article in a scholarly journal
Copyright notice ©2013, American Chemical Society
Persistent URL http://hdl.handle.net/10536/DRO/DU:30058846

Document type: Journal Article
Collection: Institute for Frontier Materials
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