Elucidation of peptide-directed palladium surface structure for biologically tunable nanocatalysts

Nicholas M. Bedford*, Hadi Ramezani-Dakhel, Joseph M. Slocik, Beverly D. Briggs, Yang Ren, Anatoly I. Frenkel, Valeri Petkov, Hendrik Heinz, Rajesh R. Naik, Marc R. Knecht

*Corresponding author for this work

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

93 Citations (Scopus)

Abstract

Peptide-enabled synthesis of inorganic nanostructures represents an avenue to access catalytic materials with tunable and optimized properties. This is achieved via peptide complexity and programmability that is missing in traditional ligands for catalytic nanomaterials. Unfortunately, there is limited information available to correlate peptide sequence to particle structure and catalytic activity to date. As such, the application of peptide-enabled nanocatalysts remains limited to trial and error approaches. In this paper, a hybrid experimental and computational approach is introduced to systematically elucidate biomolecule-dependent structure/function relationships for peptide-capped Pd nanocatalysts. Synchrotron X-ray techniques were used to uncover substantial particle surface structural disorder, which was dependent upon the amino acid sequence of the peptide capping ligand. Nanocatalyst configurations were then determined directly from experimental data using reverse Monte Carlo methods and further refined using molecular dynamics simulation, obtaining thermodynamically stable peptide-Pd nanoparticle configurations. Sequence-dependent catalytic property differences for C-C coupling and olefin hydrogenation were then elucidated by identification of the catalytic active sites at the atomic level and quantitative prediction of relative reaction rates. This hybrid methodology provides a clear route to determine peptide-dependent structure/function relationships, enabling the generation of guidelines for catalyst design through rational tailoring of peptide sequences.
Original languageEnglish
Pages (from-to)5082-5092
JournalACS Nano
Volume9
Issue number5
DOIs
Publication statusPublished - 26 May 2015
Externally publishedYes

Bibliographical note

Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

Research Keywords

  • atomic pair distribution function
  • biotemplating
  • catalysis
  • molecular dynamics simulations
  • peptides

Fingerprint

Dive into the research topics of 'Elucidation of peptide-directed palladium surface structure for biologically tunable nanocatalysts'. Together they form a unique fingerprint.

Cite this