Publication
Resolving Atomic-Scale Structure and Chemical Coordination in High Entropy Alloy Electrocatalysts for Structure-Function Relationship Elucidation
Publisher:
Research Square Platform LLC
Date:
11-2022
DOI:
10.21203/RS.3.RS-2155469/V1
Abstract: The wide range of potential surface configurations in high entropy alloy nanocatalysts (HEAs) offer substantial degrees of freedom to tune their catalytic properties. This complexity in possible atomic arrangements, however, presents a significant challenge in resolving active structural motifs, preventing the establishment of structure-function relationships for rational catalyst optimization. Herein, we present a methodology for creating sub 5 nm HEAs using an aqueous-based peptide-directed route. Using a combination of synchrotron scattering and spectroscopy techniques, HEA structure models are constructed from stochastic modelling of experimental datasets and showcase a clear peptide-induced influence on atomic-structure and chemical miscibility. Analysis of our models allow for the construction of structure-function correlations applied to electrochemical methanol oxidation reactions, revealing the complex interactions between multiple metals that lead to improved catalytic properties. Our results showcase a viable strategy for elucidating structure-function relationship in HEAs, prospectively providing a pathway for future materials design.