Time-resolved XANES investigation of CuO/ZnO in the oxidative methanol reforming reaction

T. L. Reitz, K. F. Czaplewski, J. C. Lang, K. E. Popp, H. H. Kung

Research output: Contribution to journalArticlepeer-review

130 Scopus citations

Abstract

CuO/ZnO catalysts were examined by time-resolved X-ray absorption spectroscopy during oxidative reforming of methanol. Under low oxygen conversion conditions, Cu2+ was the dominant copper species and combustion of methanol to carbon dioxide and water was the primary reaction. After complete oxygen conversion, Cu2+ was reduced to Cu0 while the principal activity of the catalyst shifted to steam reforming, where the dominant product was hydrogen. Cu+ was observed as a transient species in the reduction of Cu2+ to Cu0 and no activity was attributed to it. Increasing the oxygen partial pressure increased the rate of reduction of Cu2+. This observation was attributed to a heating effect associated with an enhancement of the combustion rate. Additional experiments showed that the catalyst could recover its original activity after a reduction/oxidation cycle.

Original languageEnglish (US)
Pages (from-to)193-201
Number of pages9
JournalJournal of Catalysis
Volume199
Issue number2
DOIs
StatePublished - 2001

Funding

The work at the Advanced Photon Source was supported by the U.S. Department of Energy under Contract No. W-31-109-ENG-38. Discus- sions on principal component analysis with S. Wasserman and assistance with the experimental setup by A. Mashayekhi and T. Middleton and financial support by Argonne National Laboratory are gratefully acknowledged.

Keywords

  • Autothermal
  • CuO/ZnO/AlO
  • Methanol
  • Oxidative reforming
  • XANES

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

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