Diferrate [Fe2 (CO)6 (μ-CO){μ-P(aryl)2 }]- as Self-Assembling Iron/Phosphor-Based Catalyst for the Hydrogen Evolution Reaction in Photocatalytic Proton Reduction-Spectroscopic Insights

Chemistry : a European Journal
Steffen FischerRalf Ludwig

Abstract

This work is focused on the identification and investigation of the catalytically relevant key iron species in a photocatalytic proton reduction system described by Beller and co-workers. The system is driven by visible light and consists of the low-cost [Fe3 (CO)12 ] as catalyst precursor, electron-poor phosphines P(R)3 as co-catalysts, and a standard iridium-based photosensitizer dissolved in a mixture of THF, water, and the sacrificial reagent triethylamine. The catalytic reaction system was investigated by operando continuous-flow FTIR spectroscopy coupled with H2 gas volumetry, as well as by X-ray absorption spectroscopy, NMR spectroscopy, DFT calculations, and cyclic voltammetry. Several iron carbonyl species were identified, all of which emerge throughout the catalytic process. Depending on the applied P(R)3 , the iron carbonyl species were finally converted into [Fe2 (CO)6 (μ-CO){μ-P(R)2 }]- . This involves a P-C cleavage reaction. The requirements of P(R)3 and the necessary reaction conditions are specified. [Fe2 (CO)6 (μ-CO){μ-P(R)2 }]- represents a self-assembling, sulfur-free [FeFe]-hydrogenase active-site mimic and shows good catalytic activity if the substituent R is electron poor. Deactivation mechanisms have als...Continue Reading

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Citations

Nov 21, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Agnieszka MielcarekAnna Dołęga
Sep 19, 2019·Faraday Discussions·Anke SchochMatthias Bauer

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