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.; Bunker, Bruce A.

doi:10.1021/acsnano.6b03963

Title: Peptide-Directed PdAu Nanoscale Surface Segregation: Toward Controlled Bimetallic Architecture for Catalytic Materials

Journal Article · Thu Sep 01 00:00:00 EDT 2016 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.6b03963· OSTI ID:1368096

Bedford, Nicholas M. ^[1]; Showalter, Allison R. ^[2]; Woehl, Taylor J. ^[1]; Hughes, Zak E. ^[3]; Lee, Sungsik ^[4]; Reinhart, Benjamin ^[4]; Ertem, S. Piril ^[5]; Coughlin, E. Bryan ^[5]; Ren, Yang ^[4]; Walsh, Tiffany R. ^[3]; Bunker, Bruce A. ^[2]

National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
Univ. of Notre Dame, IN (United States). Dept. of Physics
Deakin Univ., Geelong, Victoria (Australia). Inst. for Frontier Materials
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Sciences Division
Univ. of Massachusetts, Amherst, MA (United States). Dept. of Polymer Science and Engineering

Bimetallic nanoparticles are of immense scientific and technological interest given the synergistic properties observed when mixing two different metallic species 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 were 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 solute tempering molecular dynamic 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. Finally, 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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); Australian Government; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; FA9550-12-620 1-0226

OSTI ID:: 1368096

Journal Information:: ACS Nano, Vol. 10, Issue 9; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 49 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
atomic pair distribution function analysis
bimetallic nanoparticles
core-shell nanoparticles
electrocatalysis
peptide-enabled nanoparticles
x-ray absorption spectroscopy
x-ray diffraction

Title: Peptide-Directed PdAu Nanoscale Surface Segregation: Toward Controlled Bimetallic Architecture for Catalytic Materials

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