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Heptamolybdate: a highly active sulfide oxygenation catalyst.

Ashlin G Porter1, Hanfeng Hu, Xuemei Liu

  • 1Department of Chemistry, Purdue University, 560 Oval Drive, West Lafayette, IN 47906, USA. yxia@purdue.edu tren@purdue.edu.

Dalton Transactions (Cambridge, England : 2003)
|May 30, 2018
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Summary
This summary is machine-generated.

Heptamolybdate and its peroxo adduct catalyze sulfide oxygenation. Surprisingly, the heptamolybdate catalyst is more active than its peroxo form, with a dimeric molybdate species likely being the active catalyst.

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Area of Science:

  • Inorganic Chemistry
  • Catalysis
  • Oxidation Reactions

Background:

  • Sulfide oxygenation is crucial for synthesizing sulfoxides and sulfones.
  • Molybdate complexes are known catalysts for oxidation reactions.
  • Understanding catalytic mechanisms requires identifying active species.

Purpose of the Study:

  • To compare the sulfide oxygenation activities of heptamolybdate and its peroxo adduct.
  • To characterize the peroxo adduct and elucidate the catalytic mechanism.
  • To identify the active species in heptamolybdate-catalyzed sulfide oxygenation.

Main Methods:

  • Synthesis and structural characterization of the peroxo adduct using single crystal X-ray diffraction.
  • Catalytic oxidation of methyl phenyl sulfide (MPS) using hydrogen peroxide.
  • Kinetic studies to determine rate constants (kcat).
  • Electrospray ionization mass spectrometry (ESI-MS) to identify active species.

Main Results:

  • The peroxo adduct [Mo7O22(O2)2]6- was synthesized and structurally identified.
  • Both heptamolybdate ([Mo7O24]6-) and its peroxo adduct catalyzed sequential MPS oxygenation to sulfoxide and sulfone with high H2O2 utility.
  • Heptamolybdate ([Mo7O24]6-) exhibited significantly higher catalytic activity than the peroxo adduct.
  • ESI-MS suggested [Mo2O11]2- as the likely active species for heptamolybdate.

Conclusions:

  • Heptamolybdate is a more effective catalyst for MPS oxygenation than its peroxo adduct.
  • The catalytic activity is linked to the formation of a dimeric molybdate species.
  • This study provides insights into the mechanism of molybdate-catalyzed sulfide oxygenation.