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[ReH(SH)2 (PMe3 )4 ]: A Catalyst for Fundamental Transformations Involving H2 and H2 S.

Daniel E Schwarz1, Joel A Dopke1, Thomas B Rauchfuss1

  • 1School of Chemical Sciences University of Illinois Urbana, IL 61801 (USA) Fax: (+1) 217-333-2685.

Angewandte Chemie (International Ed. in English)
|May 2, 2018
PubMed
Summary

Sulfur compounds do not poison catalysts as previously thought. Instead, the difunctional nature of compound 1, featuring both protic (SH) and hydridic (ReH) sites, enables its catalytic properties through intramolecular communication.

Keywords:
P ligandshomogeneous catalysishydrodesulfurizationhydrogenrheniumsulfur

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Area of Science:

  • Organometallic Chemistry
  • Catalysis
  • Inorganic Chemistry

Background:

  • The reactivity of organosulfur compounds in catalysis is often viewed negatively, with sulfur typically considered a catalyst poison.
  • The kinetic inertness of the trihydride [ReH3(PMe3)4] contrasts with the high reactivity of related compounds, prompting a re-evaluation of sulfur's role.

Purpose of the Study:

  • To investigate the catalytic properties of compound 1, specifically challenging the notion of sulfur as a catalyst poison.
  • To elucidate the mechanism behind the catalytic activity of compound 1, focusing on its unique structural and electronic features.

Main Methods:

  • Synthesis and characterization of the trihydride complex [ReH3(PMe3)4].
  • Kinetic studies to assess the inertness of the trihydride complex.
  • Investigation of the catalytic behavior of compound 1, examining its difunctional nature.

Main Results:

  • The trihydride [ReH3(PMe3)4] exhibits kinetic inertness, contradicting the general assumption of sulfur poisoning.
  • Compound 1 demonstrates catalytic activity, attributed to its difunctional nature.
  • An intramolecular exchange process between protic (SH) and hydridic (ReH) sites in compound 1 was identified as key to its catalytic function.

Conclusions:

  • The traditional view of sulfur as a catalyst poison is inappropriate for compound 1.
  • The catalytic efficacy of compound 1 stems from the interplay between its protic and hydridic functionalities.
  • Intramolecular communication between SH and ReH sites is crucial for the observed catalytic properties.