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Solvation effects on transition metal hydricity.

Charlene Tsay1, Brooke N Livesay1, Samantha Ruelas1

  • 1Department of Chemistry, University of California , Irvine, California 92697, United States.

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|October 15, 2015
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Summary

This study reports the first hydricity values for a transition metal hydride in various solvents. Increasing solvent polarity narrows the range of hydricity values, impacting hydride transfer reactions.

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Area of Science:

  • Organometallic Chemistry
  • Physical Chemistry
  • Catalysis

Background:

  • Hydricity, the free energy of hydride donation, is crucial for understanding hydride transfer reactions.
  • Transition metal hydrides are important in catalysis, but their hydricity in different solvents is not well-documented.

Purpose of the Study:

  • To experimentally determine the hydricity of a specific transition metal hydride, [HNi(DHMPE)2][BF4], in three different solvents.
  • To compare these values with known hydricity data for hydrogen and formate.
  • To investigate the influence of solvent polarity on hydricity and hydride transfer thermodynamics.

Main Methods:

  • Experimental determination of the free energy of hydride donation (hydricity).
  • Measurement of heterolytic cleavage energy of hydrogen in acetonitrile, dimethyl sulfoxide, and water.
  • Comparative analysis of hydricity values across different solvents and with other hydride donors.

Main Results:

  • Hydricity values for [HNi(DHMPE)2][BF4] were determined as 57.4 kcal/mol (acetonitrile), 55.5 kcal/mol (dimethyl sulfoxide), and 30.0 kcal/mol (water).
  • A narrowing range of hydricity values was observed with increasing solvent polarity.
  • Solvation effects significantly impact the thermodynamic favorability of hydride generation and transfer.

Conclusions:

  • The study provides the first hydricity data for a transition metal hydride in multiple solvents.
  • Solvent polarity plays a critical role in modulating hydricity and influencing hydride transfer processes.
  • These findings have implications for designing catalysts involved in hydride transfer reactions in synthetic chemistry.