Form of the catalytically active Pd species during the direct synthesis of hydrogen peroxide

Pranjali Priyadarshini, David W. Flaherty

Research output: Contribution to journalArticlepeer-review

Abstract

Direct synthesis of H2O2 could produce H2O2 at lower cost than the Riedl–Pfleiderer process, which would enable the broader use of H2O2 for industrial oxidations. The addition of inorganic acids and halides to the solvent increase H2O2 selectivities on Pd nanoparticles but also dissolve Pd and produce dynamic mixtures of complexes including heterogeneous (Pd0) and homogeneous (Pd2+) species, any of which may contribute to H2O2 formation. We combine kinetic measurements and in operando UV–vis spectroscopy to determine how H2O2 rates and selectivities depend on concentrations of these forms of Pd. Introducing HCl to the solvent increases the concentration of Pd2+ complexes by oxidizing Pd0 nanoparticles. The rates of primary H2O2 formation and H2O2 selectivities do not depend directly on the population of the Pd2+ species for catalysts tested in water or methanol. These results suggest that Pd nanoparticles form H2O2 and detectable homogeneous complexes do not act as catalysts.

Original languageEnglish (US)
Article numbere16829
JournalAIChE Journal
Volume65
Issue number12
DOIs
StatePublished - Dec 1 2019

Keywords

  • catalysis
  • corrosion
  • spectroscopy

ASJC Scopus subject areas

  • Biotechnology
  • Environmental Engineering
  • Chemical Engineering(all)

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