Observation and Identification of an Atomic Oxygen Structure on Catalytic Gold Nanoparticles

Kai Liu, Tao Chen, Shuyue He, Jason P. Robbins, Simon G. Podkolzin, Fei Tian

Research output: Contribution to journalArticlepeer-review

32 Scopus citations

Abstract

Interactions between oxygen and gold surfaces are fundamentally important in diverse areas of science and technology. In this work, an oxygen dimer structure was observed and identified on gold nanoparticles in catalytic decomposition of hydrogen peroxide to oxygen and water. This structure, which is different from isolated atomic or molecular oxygen surface structures, was observed with in situ surface-enhanced Raman spectroscopic measurements and identified with density functional theory calculations. The experimental measurements were performed using monodisperse 5, 50 and 400 nm gold particles supported on silica with liquid-phase hydrogen and deuterium peroxides at multiple pH values. The calculations show that on surfaces with coordinatively unsaturated gold atoms, two oxygen atoms preferentially share a gold atom with a bond distance of 0.194–0.196 nm and additionally bind to two other surface gold atoms with a larger bond distance of 0.203–0.213 nm, forming an Au-O-Au-O-Au structure. The formation of this structure depends on reaction rates and conditions.

Original languageEnglish
Pages (from-to)12952-12957
Number of pages6
JournalAngewandte Chemie - International Edition
Volume56
Issue number42
DOIs
StatePublished - 9 Oct 2017

Keywords

  • Au surface
  • HO decomposition
  • adsorbed oxygen
  • kinetic measurements
  • monodisperse nanoparticles

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