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Non‐covalent integration of a [FeFe]‐hydrogenase mimic to multiwalled carbon nanotubes for electrocatalytic hydrogen evolution

Von Wiley-VCH zur Verfügung gestellt

Surface integration of molecular catalysts inspired from the active sites of hydrogenase enzymes represents a promising route towards developing noble metal-free and sustainable technologies for H 2 production. Efficient and stable catalyst anchoring is a key aspect to enable this approach. Here, we report the preparation and electrochemical characterization of an original diironhexacarbonyl complex including two pyrene groups per catalytic unit in order to allow for its smooth integration, through pi-pi  interactions, onto MWNT based electrodes. In this configuration, the grafted catalyst could reach turnover numbers for H 2 production (TON H2 ) of up to 3.5 ± 1.6 x 10 3 within 20 hours of bulk electrolysis, operating at neutral pH. Post operando analysis of catalyst func­tionalized electrodes revealed the degradation of the catalytic unit occurred via loss of the Fe 2 (CO) 6 units, while the anchoring groups and most part of the ligand remained attached onto MWNT.

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