Proceedings of nanoGe Fall Meeting19 (NFM19)
DOI: https://doi.org/10.29363/nanoge.nfm.2019.081
Publication date: 18th July 2019
Very fast oxygen reduction catalyzed by Cu(tmpa); Towards hydrogen peroxide as a solar fuel
For an energy transition from a fuel based economy to an economy that is based on solar and wind energy that suffer from intermittency problems it is important to be able to convert electricity into chemical fuels. Besides the production of hydrogen, lately also electrochemical reduction of carbon dioxide and dinitrogen have been of interest to the scientific community. The use of hydrogen peroxide as a fuel, on the other hand, has thus far been overlooked. In part this is due to a lack of good and selective catalysts for the electrochemical synthesis of hydrogen peroxide.
My group has recently shown that hydrogen peroxide can be obtained at the cathode with more than 90% faradaic efficiency using the molecular catalyst Cu(tmpa).[1] Under optimized conditions the catalyst operates with more than a million turnovers per second, and with an onset at a 200 mV overpotential. The catalytic currents are limited by mass transport of buffer and oxygen concentrations.
The key to selectivity lies in that Cu(tmpa) is a single site catalysts that is very limited in how many electrons it can deliver to the substrate simultaneously. In addition ligand exchange reactions, including the dissociation of hydrogen peroxide, are very rapid while Karlin et al. have already established that oxygen binding to Cu(I) occurs through a very rapid reaction.[2]
At the lecture the precise mechanism towards hydrogen peroxide synthesis, bulk electrolysis results and in situ spectroscopy of the H2O2 synthesis will be discussed.
References
[1] M. Langerman, D. G. H. Hetterscheid, Angew. Chem., Int. Ed., DOI: 10.1002/anie.201904075
[2] H. C. Fry, D. V. Scaltrito, K. D. Karlin, G. J. Meyer, J. Am. Chem. Soc. 2003, 125, 11866-11871
The European Research Council (ERC) is acknowledged for the funding of this project (ERC starting grant 637556 Cu4Energy to D. G. H. H.).
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