Proceedings of Online nanoGe Fall Meeting 20 (OnlineNFM20)
Publication date: 4th October 2020
Rational design and comparative studies of catalysts rely on detailed information about the mechanism of catalysis that in most cases is not available. We have used time-resolved UV/VIS and mid-IR spectroscopy to resolve highly reactive catalyst intermediates on the nano- to millisecond time scale, elucidate their structures and measure their reactivity in proton- and electron transfer reactions of the mechanistic cycle [1].
The azadithiolate bridge of FeFe-hydrogenase active sites has been taken as an example design for proton relays in the second coordination sphere, facilitating protonation and deprotonation of the metal centre. We have shown that for the corresponding model complexes, the aza-group has no role as proton shuttle in the FeIFe0 state, as had been proposed [2]. Instead, the effect of aza protonation is to shift the catalyst reduction potential, surprisingly with no or only little reduction in the rate of subsequent metal protonation by external acid.
We have also been able to follow the charge transfer dynamics via mid-IR signals of the catalyst in catalyst-semiconductor systems, with both band-gap excitation and dye-sensitization. Ultra-fast (<300 fs) catalyst reduction of molecular catalysts for CO2 or proton reduction is observed on CuInS2 quantum dots ([3] and manuscript in progress).
Support from the Swedish Research Council and the Swedish Energy Agency is greatfully Acnowledged
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