Abstract

The development of single site electrocatalysts such as single-atom catalyst (SAC) has demonstrated the advantages of high precious metal utilization and tunable metal-support interfacial properties. However, the fundamental understanding of unalloyed single metal atom decorated on a metallic substrate is still lacking. Herein, we report unalloyed single atomic, partially oxidized Rh on the Pt nanocube surface as the electrocatalyst to completely oxidize ethanol to CO2at a record-low potential of 0.35 V. In situ X-ray absorption fine structure measurements and density functional theory calculations reveal that the single-atom Rh sites facilitate the C-C bond cleavage and the removal of the *CO intermediates. This work not only reveals the fundamental role of unalloyed, partially oxidized SAC in ethanol oxidation reaction but also offers a unique single-atom approach using low-coordination active sites on shape-controlled nanocatalysts to tune the activity and selectivity toward complicated catalytic reactions.

Original languageEnglish
Article numbere2112109119
JournalProceedings of the National Academy of Sciences of the United States of America
Volume119
Issue number11
DOIs
StatePublished - 15 Mar 2022

Keywords

  • ethanol oxidation reaction
  • platinum nanocubes
  • rhodium
  • single atom catalyst

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