Abstract
The tetrahedral copper(I) diimine complex [Cu(pq)2]BF4 displays high photocatalytic activity for the H2 evolution reaction with a turnover number of 3564, thus representing the first type of a Cu(I) quinoxaline complex capable of catalyzing proton reduction. Electrochemical experiments indicate that molecular mechanisms prevail and DFT calculations provide in-depth insight into the catalytic pathway, suggesting that the coordinating nitrogens play crucial roles in proton exchange and hydrogen formation.
Highlights
Copper catalysts for proton reduction have recently gained special attention in facilitating solar and electrochemical energy storage via the formation of hydrogen fuel
We have presented that the Cu(I) diimine complex [1]+ can serve as a molecular photocatalyst for water reduction in combination with fluorescein as a photosensitizer and triethanolamine as a sacrificial electron donor achieving 3564 turnovers, after 24h of irradiation
We have presented that the Cu(I) diimine complex [1]+ can serve as a molecular photocatalyst for water reduction in combination with fluorescein as a photosensitizer and triethanolamine as a sacrificial electron donor achieving 3564 turnovers, after 24 h of irradiation
Summary
Copper catalysts for proton reduction have recently gained special attention in facilitating solar and electrochemical energy storage via the formation of hydrogen fuel. Distorted trigonal bipyramidal and square pyramidal Cu(II) complexes bearing polypyridine chelates, which are supposed to minimize the inherent lability of the d10 Cu(I) ion, have been extensively explored as proton reduction electrocatalysts and photocatalysts. Their proposed catalytic pathways involve proton coupled electron transfer (PCET) processes leading to a Cu(II)-hydride that evolves H2 via intramolecular coupling between the hydride and the proton of a pendant pyridine nitrogen [24,25,26,27]
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