Peptide-directed PdAu nanoscale surface segregation: toward controlled bimetallic architecture for catalytic materials

Bedford, Nicholas M., Showalter, Allison R., Woehl, Taylor J., Hughes, Zak E., Lee, Sungsik, Reinhart, Benjamin, Ertem, S. Piril, Coughlin, E. Bryan, Ren, Yang, Walsh, Tiffany R. and Bunker, Bruce A. 2016, Peptide-directed PdAu nanoscale surface segregation: toward controlled bimetallic architecture for catalytic materials, ACS nano, vol. 10, no. 9, pp. 8645-8659, doi: 10.1021/acsnano.6b03963.

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Title Peptide-directed PdAu nanoscale surface segregation: toward controlled bimetallic architecture for catalytic materials
Author(s) Bedford, Nicholas M.
Showalter, Allison R.
Woehl, Taylor J.
Hughes, Zak E.ORCID iD for Hughes, Zak E.
Lee, Sungsik
Reinhart, Benjamin
Ertem, S. Piril
Coughlin, E. Bryan
Ren, Yang
Walsh, Tiffany R.ORCID iD for Walsh, Tiffany R.
Bunker, Bruce A.
Journal name ACS nano
Volume number 10
Issue number 9
Start page 8645
End page 8659
Total pages 15
Publisher American Chemical Society
Place of publication Washington D.C.
Publication date 2016
ISSN 1936-086X
Keyword(s) X-ray absorption spectroscopy
atomic pair distribution function analysis
bimetallic nanoparticles
peptide-enabled nanoparticles
Science & Technology
Physical Sciences
Chemistry, Multidisciplinary
Chemistry, Physical
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Science & Technology - Other Topics
Materials Science
Summary Bimetallic nanoparticles are of immense scientific and technological interest given the synergistic properties observed when two different metallic species are mixed at the nanoscale. This is particularly prevalent in catalysis, where bimetallic nanoparticles often exhibit improved catalytic activity and durability over their monometallic counterparts. Yet despite intense research efforts, little is understood regarding how to optimize bimetallic surface composition and structure synthetically using rational design principles. Recently, it has been demonstrated that peptide-enabled routes for nanoparticle synthesis result in materials with sequence-dependent catalytic properties, providing an opportunity for rational design through sequence manipulation. In this study, bimetallic PdAu nanoparticles are synthesized with a small set of peptides containing known Pd and Au binding motifs. The resulting nanoparticles were extensively characterized using high-resolution scanning transmission electron microscopy, X-ray absorption spectroscopy, and high-energy X-ray diffraction coupled to atomic pair distribution function analysis. Structural information obtained from synchrotron radiation methods was then used to generate model nanoparticle configurations using reverse Monte Carlo simulations, which illustrate sequence dependence in both surface structure and surface composition. Replica exchange with solute tempering molecular dynamics simulations were also used to predict the modes of peptide binding on monometallic surfaces, indicating that different sequences bind to the metal interfaces via different mechanisms. As a testbed reaction, electrocatalytic methanol oxidation experiments were performed, wherein differences in catalytic activity are clearly observed in materials with identical bimetallic composition. Taken together, this study indicates that peptides could be used to arrive at bimetallic surfaces with enhanced catalytic properties, which could be leveraged for rational bimetallic nanoparticle design using peptide-enabled approaches.
Language eng
DOI 10.1021/acsnano.6b03963
Field of Research 100708 Nanomaterials
100706 Nanofabrication, Growth and Self Assembly
091205 Functional Materials
030406 Proteins and Peptides
030601 Catalysis and Mechanisms of Reactions
MD Multidisciplinary
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, American Chemical Society
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