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

Abstract

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 differentmore » 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.« less

Authors:
 [1];  [2];  [1];  [3];  [4];  [4];  [5];  [5];  [4];  [3];  [2]
+ Show Author Affiliations
  1. National Inst. of Standards and Technology (NIST), Boulder, CO (United States)
  2. Univ. of Notre Dame, IN (United States). Dept. of Physics
  3. Deakin Univ., Geelong, Victoria (Australia). Inst. for Frontier Materials
  4. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Sciences Division
  5. Univ. of Massachusetts, Amherst, MA (United States). Dept. of Polymer Science and Engineering
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); Australian Government; National Science Foundation (NSF)
OSTI Identifier:
1368096
Grant/Contract Number:  
AC02-06CH11357; FA9550-12-620 1-0226
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 10; Journal Issue: 9; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
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

Citation Formats

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. Peptide-Directed PdAu Nanoscale Surface Segregation: Toward Controlled Bimetallic Architecture for Catalytic Materials. United States: N. p., 2016. Web. doi:10.1021/acsnano.6b03963.
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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. Peptide-Directed PdAu Nanoscale Surface Segregation: Toward Controlled Bimetallic Architecture for Catalytic Materials. United States. https://doi.org/10.1021/acsnano.6b03963
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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. Thu . "Peptide-Directed PdAu Nanoscale Surface Segregation: Toward Controlled Bimetallic Architecture for Catalytic Materials". United States. https://doi.org/10.1021/acsnano.6b03963. https://www.osti.gov/servlets/purl/1368096.
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@article{osti_1368096,
title = {Peptide-Directed PdAu Nanoscale Surface Segregation: Toward Controlled Bimetallic Architecture for Catalytic Materials},
author = {Bedford, Nicholas M. and Showalter, Allison R. and Woehl, Taylor J. and Hughes, Zak E. and Lee, Sungsik and Reinhart, Benjamin and Ertem, S. Piril and Coughlin, E. Bryan and Ren, Yang and Walsh, Tiffany R. and Bunker, Bruce A.},
abstractNote = {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.},
doi = {10.1021/acsnano.6b03963},
journal = {ACS Nano},
number = 9,
volume = 10,
place = {United States},
year = {Thu Sep 01 00:00:00 EDT 2016},
month = {Thu Sep 01 00:00:00 EDT 2016}
}
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    • Dalton Transactions, Vol. 46, Issue 35
    • DOI: 10.1039/c7dt02095c

    Hemi-core@frame AuCu@IrNi nanocrystals as active and durable bifunctional catalysts for the water splitting reaction in acidic media
    journal, January 2019

    • Park, Jongsik; Choi, Songa; Oh, Aram
    • Nanoscale Horizons, Vol. 4, Issue 3
    • DOI: 10.1039/c8nh00520f

    Oligomerization enhances the binding affinity of a silver biomineralization peptide and catalyzes nanostructure formation
    journal, May 2017

    • Sakaguchi, Tatsuya; Janairo, Jose Isagani B.; Lussier-Price, Mathieu
    • Scientific Reports, Vol. 7, Issue 1
    • DOI: 10.1038/s41598-017-01442-8
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