Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.189
Publication date: 7th February 2022
Carbon dioxide reduction by porphrynic metal-organic frameworks has been widely studied. Changes in porphyrin moiety (non-metallated, different central metal atoms) and three-dimensional structures result in putative changes in mechanism and resulting products, namely carbon monoxide and formate. There are two prevailing mechanisms that are debated in the literature (1) the formation of a porphyrin-node charge-separated state, where the node acts as the catalytic site, (2) porphyrin driven chemistry where the linker acts as both the photo-active species and catalytic site with the nodes simply serving as structural supports. Our collaborators have systematically explored the reduction rates and products for different non-metallated and metallated MOF-525. To support the mechanistic implications, we conducted photophysical studies, including transient absorption spectroscopy. Interestingly, the results do not support either of the prevailing mechanisms. Transient absorption spectroscopy eliminates the possibility for the formation of a charge-separated state. EPR spectroscopy confirms that the photogenerated Fe(II) species is not capable of carbon dioxide activation, consistent with previously published molecular mechanisms. Therefore, we turned to theory to provide insight. The computational results support a mechanism where the sacrificial donor plays a key role in the catalytic mechanism. Other recent mechanistic studies on molecular carbon dioxide reduction catalysts have put forth similar stories with sacrificial donors playing multiple roles in catalysis. The implications of sacrificial reducing agents in the field will be mentioned, as well as potential pathways for future research.
This research was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award DE-SC0012445.
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