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Switchable molecular electrocatalysis.

Shifali Dutt1, Alagar Raja Kottaichamy1,2, Neethu Christudas Dargily1

  • 1Department of Chemistry, Indian Institute of Science Education and Research (IISER)-Pune Dr Homi Bhabha Road, Pashan Pune 411008 Maharashtra India musthafa@iiserpune.ac.in.

Chemical Science
|August 26, 2024
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Summary
This summary is machine-generated.

Ligand geometry controls electrocatalysis, switching between dioxygen electroreduction (ORR) and hydrogen evolution (HER). This discovery offers a new paradigm for selective molecular electrocatalysis by manipulating hydrogen bonding interactions.

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Area of Science:

  • Molecular electrocatalysis
  • Coordination chemistry
  • Electrochemical energy conversion

Background:

  • Ligand design is crucial for controlling catalytic activity in molecular electrocatalysis.
  • Understanding structure-activity relationships is key to developing efficient electrocatalysts.
  • Hydrogen bonding interactions can significantly influence electronic properties and reactivity.

Purpose of the Study:

  • To demonstrate a switchable electrocatalysis mechanism modulated by ligand geometry and hydrogen bonding.
  • To investigate the selective activation/deactivation of electrochemical processes at a single catalytic site.
  • To explore the distinct roles of different ligand geometries (α and β) in dioxygen electroreduction (ORR) and hydrogen evolution (HER).

Main Methods:

  • Synthesis and characterization of metal complexes with varying ligand geometries.
  • Electrochemical studies to evaluate catalytic activity for ORR and HER.
  • Computational analysis to understand the electronic effects of ligand geometry and hydrogen bonding.

Main Results:

  • The α geometry selectively enhances 4-electron ORR by increasing electron density at the catalytic center via intramolecular hydrogen bonding.
  • The β geometry promotes 2-electron ORR and facilitates HER through proton charge assembly.
  • Contrasting reactivity observed between α and β geometries challenges conventional electrocatalytic principles.

Conclusions:

  • Ligand geometry is a powerful tool for controlling electrocatalytic pathways, offering switchable mechanisms.
  • Hydrogen bonding plays a critical role in modulating electron density and catalytic performance.
  • This work provides a new paradigm for designing selective molecular electrocatalysts for energy applications.