Sequence-dependent structure/function relationships of catalytic peptide-enabled gold nanoparticles generated under ambient synthetic conditions

Bedford, Nicholas M., Hughes, Zak E., Tang, Zhenghua, Li, Yue, Briggs, Beverly D., Ren, Yang, Swihart, Mark T., Petkov, Valeri G., Naik, Rajesh R., Knecht, Marc R. and Walsh,Tiffany R. 2016, Sequence-dependent structure/function relationships of catalytic peptide-enabled gold nanoparticles generated under ambient synthetic conditions, Journal of the American chemistry society, vol. 138, no. 2, pp. 540-548, doi: 10.1021/jacs.5b09529.

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Title Sequence-dependent structure/function relationships of catalytic peptide-enabled gold nanoparticles generated under ambient synthetic conditions
Author(s) Bedford, Nicholas M.
Hughes, Zak E.ORCID iD for Hughes, Zak E.
Tang, Zhenghua
Li, Yue
Briggs, Beverly D.
Ren, Yang
Swihart, Mark T.
Petkov, Valeri G.
Naik, Rajesh R.
Knecht, Marc R.
Walsh,Tiffany R.ORCID iD for Walsh,Tiffany R.
Journal name Journal of the American chemistry society
Volume number 138
Issue number 2
Start page 540
End page 548
Total pages 9
Publisher ACS Publications
Place of publication Washington, D.C.
Publication date 2016
ISSN 1520-5126
Keyword(s) Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Summary Peptide-enabled nanoparticle (NP) synthesis routes can create and/or assemble functional nanomaterials under environmentally friendly conditions, with properties dictated by complex interactions at the biotic/abiotic interface. Manipulation of this interface through sequence modification can provide the capability for material properties to be tailored to create enhanced materials for energy, catalysis, and sensing applications. Fully realizing the potential of these materials requires a comprehensive understanding of sequence-dependent structure/function relationships that is presently lacking. In this work, the atomic-scale structures of a series of peptide-capped Au NPs are determined using a combination of atomic pair distribution function analysis of high-energy X-ray diffraction data and advanced molecular dynamics (MD) simulations. The Au NPs produced with different peptide sequences exhibit varying degrees of catalytic activity for the exemplar reaction 4-nitrophenol reduction. The experimentally derived atomic-scale NP configurations reveal sequence-dependent differences in structural order at the NP surface. Replica exchange with solute-tempering MD simulations are then used to predict the morphology of the peptide overlayer on these Au NPs and identify factors determining the structure/catalytic properties relationship. We show that the amount of exposed Au surface, the underlying surface structural disorder, and the interaction strength of the peptide with the Au surface all influence catalytic performance. A simplified computational prediction of catalytic performance is developed that can potentially serve as a screening tool for future studies. Our approach provides a platform for broadening the analysis of catalytic peptide-enabled metallic NP systems, potentially allowing for the development of rational design rules for property enhancement.
Language eng
DOI 10.1021/jacs.5b09529
Field of Research 030302 Nanochemistry and Supramolecular Chemistry
030601 Catalysis and Mechanisms of Reactions
030406 Proteins and Peptides
030603 Colloid and Surface Chemistry
030704 Statistical Mechanics in Chemistry
03 Chemical Sciences
Socio Economic Objective 970103 Expanding Knowledge in the Chemical Sciences
HERDC Research category C1 Refereed article in a scholarly journal
ERA Research output type C Journal article
Copyright notice ©2016, ACS Publications
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