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Title: Elucidation of Peptide-Directed Palladium Surface Structure for Biologically Tunable Nanocatalysts

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 eluddated 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
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Publication Date:
OSTI Identifier:
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Nano; Journal Volume: 9; Journal Issue: 5
American Chemical Society
Research Org:
Argonne National Laboratory (ANL)
Sponsoring Org:
Argonne National Laboratory - Advanced Photon Source; Air Force Research Laboratory - Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); National Research Council; USDOE Office of Science - Office of Basic Energy Sciences
Country of Publication:
United States
atomic pair distribution function; bio-templating; catalysis; molecular dynamics simulations; peptides