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Mononuclear Fe(III) Schiff base antipyrine complexes for catalytic hydrogen generation
Jessica D Cropley1, Amanda C Mitchell1, Nicole A Fritsch1
1Department of Chemistry, College of William and Mary, 540 Landrum Drive, Williamsburg, VA 23185, USA. wrmcnamara@wm.edu.
New iron complexes act as efficient electrocatalysts for hydrogen evolution, achieving high turnover frequencies. These catalysts also show promise in photocatalysis and function in natural water samples.
Area of Science:
- Inorganic Chemistry
- Catalysis
- Materials Science
Background:
- Mononuclear iron(III) complexes are crucial in catalysis.
- Schiff base ligands offer versatile coordination environments.
- Hydrogen evolution reaction (HER) is a key process for sustainable energy.
Purpose of the Study:
- To synthesize and characterize novel mononuclear Fe(III) complexes with antipyrine Schiff base ligands.
- To evaluate the electrocatalytic and photocatalytic activity of these complexes for hydrogen production.
- To assess the stability and performance of the catalysts in varying environmental conditions.
Main Methods:
- Synthesis and full characterization of Fe(III) complexes.
- Electrochemical studies including cyclic voltammetry and chronoamperometry.
- Photocatalytic experiments using a chromophore and sacrificial donor.
- Catalyst performance evaluation in natural water samples.
Main Results:
- Complexes exhibit a planar tetradentate coordination geometry.
- Electrocatalytic hydrogen evolution occurs at -1.4 V vs. Fc+/Fc with 700 mV overpotential and a turnover frequency of 700 s⁻¹.
- Photocatalytic activity demonstrated >1700 turnovers over 40 hours with a quantum yield up to 5.4%.
- Catalysts maintain activity in natural water samples with diverse salinity.
Conclusions:
- The synthesized Fe(III) complexes are effective electrocatalysts and photocatalysts for hydrogen evolution.
- These complexes show potential for application in sustainable hydrogen production technologies.
- The catalysts' robustness in natural water environments highlights their practical applicability.
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