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A new potentiometric method quantifies hydride transfer (ΔGH-) for challenging main group reagents. This HRR potentiometry approach offers insights into reaction environments and reagent behavior, expanding hydricity measurement capabilities.

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Area of Science:

  • Chemistry
  • Electrochemistry
  • Physical Chemistry

Background:

  • Hydride transfer is crucial in chemical processes, but quantifying thermodynamic hydricity (ΔGH-) is challenging for main group reagents.
  • Existing methods for measuring hydricity are limited, especially for reagents resistant to conventional techniques.

Purpose of the Study:

  • To develop and validate a novel potentiometric method, HRR potentiometry, for quantifying the thermodynamic hydricity of main group reagents.
  • To investigate the influence of reaction environments, such as solvents and water content, on the hydricity of various hydride donors.
  • To explore the impact of Lewis acid-base adduct formation and countercations on the effective hydricity of borohydrides.

Main Methods:

  • Exploitation of H2 activation and reversible hydride transfer from a metal surface to a molecular reagent (net hydrogen reduction reaction, HRR).
  • Development of a potentiometric technique (HRR potentiometry) to measure equilibrium potentials related to hydride transfer.
  • Validation of the method using a benzimidazole-based hydride donor and application to formate and borohydride systems.

Main Results:

  • HRR potentiometry successfully quantified ΔGH- for main group reagents recalcitrant to other methods.
  • Solvent effects on the hydricity of a benzimidazole-based donor were primarily attributed to differential H- solvation.
  • Formate hydricity showed strong dependence on water content, while borohydride effective hydricity was influenced by adduct formation but not countercations.

Conclusions:

  • HRR potentiometry is a powerful complementary tool for measuring molecular hydricity, offering advantages for challenging substrates.
  • The study elucidates the environmental factors affecting hydride transfer reactions and provides a reliable method for their quantification.
  • This work expands the toolkit for studying fundamental chemical reactions relevant to catalysis and energy storage.