4.8 Article

Metal-Metal Oxide Catalytic Interface Formation and Structural Evolution: A Discovery of Strong Metal-Support Bonding, Ordered Intermetallics, and Single Atoms


Volume -, Issue -, Pages -


DOI: 10.1021/acs.nanolett.2c02568


metal-metal oxide interface; strong metal-support interaction; single atoms; intermetallics; acetylene semihydrogenation


  1. ACS petroleum research foundation
  2. National Research Foundation (NRF) Singapore [NRF-NRFF11-2019-0002]
  3. Singapore Low-carbon energy research funding initiative [LCERFI01-0017]
  4. Green Energy Flagship Program in the National University of Singapore [A-0005323-09-00]
  5. DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]

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This study investigates the interactions between metal and metal oxide, revealing different behaviors among Pd, Pt, and Au nanoparticles coated with FeOx. The results show strong interactions between Pd and FeOx, while Pt forms ordered PtFe intermetallics and Au does not show strong bonding with FeOx.
In-depth investigation of metal-metal oxide inter-actions and their corresponding evolution is of paramount importance to heterogeneous catalysis as it allows the under-standing and maneuvering of the structure of catalytic motifs. Herein, using a series of core/shell metal/iron oxide (M/FeOx, M = Pd, Pt, Au) nanoparticles and through a combination of in situ and ex situ electron and X-ray investigations, we revealed anomalous and dissimilar M-FeOx interactions among different systems under reducing conditions. Pd interacts strongly with FeOx after high-temperature reductive treatment, featured by the formation of Pd single atoms in the FeOx matrix and increased Pd-Fe bonding, while Pt transforms into ordered PtFe intermetallics and Pt single atoms immediately upon the coating of FeOx. In contrast, Au does not manifest strong bonding with FeOx. As a proof of concept of tailoring metal-metal oxide interactions for catalysis, optimized Pd/FeOx demonstrates 100% conversion and 86.5% selectivity at 60 degrees C for acetylene


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