Low-Temperature Oxidation of Methanol to Formaldehyde on a Model Single-Atom Catalyst: Pd Atoms on Fe3O4(001)

Matthew D. Marcinkowski, Simuck F. Yuk, Nassar Doudin, R. Scott Smith, Manh Thuong Nguyen, Bruce D. Kay, Vassiliki Alexandra Glezakou, Roger Rousseau, Zdenek Dohnálek

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2 Citations (Scopus)

Abstract

Single-atom catalysis has been a topic of increasing interest due to the potential for improved selectivity, reactivity, and catalyst cost. However, single-atom catalysts are still difficult to characterize under realistic reaction conditions, leading to controversy regarding the capabilities of single atoms and a need for model studies. Herein, we examine the reaction of methanol on single Pd atoms supported on Fe3O4(001) under ultrahigh vacuum conditions. On Pd-free Fe3O4(001), a small fraction of methanol is converted to formaldehyde through a methoxy intermediate at 516 K. The addition of single Pd atoms lowers the barrier to C-H bond cleavage by a factor of 2, resulting in formaldehyde desorption by 290 K. However, Pd atoms begin to sinter by 300 K in the presence of methanol, and Pd clusters do not exhibit the same chemistry. Single atoms significantly lower the barrier to the oxidation of methanol, although their stability remains an issue.

Original languageEnglish
Pages (from-to)10977-10982
Number of pages6
JournalACS Catalysis
DOIs
Publication statusPublished - Jan 1 2019

Keywords

  • FeO(001)
  • heterogeneous catalysis
  • methanol
  • palladium
  • partial oxidation
  • single-atom catalysis

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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    Marcinkowski, M. D., Yuk, S. F., Doudin, N., Smith, R. S., Nguyen, M. T., Kay, B. D., Glezakou, V. A., Rousseau, R., & Dohnálek, Z. (2019). Low-Temperature Oxidation of Methanol to Formaldehyde on a Model Single-Atom Catalyst: Pd Atoms on Fe3O4(001). ACS Catalysis, 10977-10982. https://doi.org/10.1021/acscatal.9b03891