Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
Publication date: 18th July 2023
Nitrate pollution of soils and water bodies caused by intensive agriculture has become a pervasive global problem. While the input of fertilizers increased by 800 % during the last 50 years, eutrophication of lakes, ponds and coastal water bodies is now a serious biodiversity threat and a primary water quality issue.[1]
The development of new processes to remove nitrate from polluted water is crucial to address this environmental crisis, and a unique source of inspiration for the design of artificial catalysts can be found in enzymes. Dissimilatory nitrate reductase catalyzes the two-electron reduction of nitrate to nitrite and consists of a molybdopterin active site and a chain of [Fe4S4] clusters.[2] The efficiency of the enzymes lies in the powerful combination of a binding site and an electron supply chain in close vicinity. Combining electron relays with potent Lewis acidic site hence has the potential to generate bio-inspired catalysts capable of pre-activating the substrate while providing the electrons necessary for reduction. Trivalent lanthanide ions are hard Lewis acids and are therefore candidates of choice for the reduction of substrates such as NO3-. Contrary to other Lewis acids such as early transition metals, they are stable towards hydrolysis and therefore suitable for applications in water. Due to their large coordination sphere, they can accommodate multiple ligands to store electrons. Additionally, tetrathiometallates can act as convenient electron storage and relay sites by accepting electron density in low-lying, empty d orbitals.[3] Consequently, we developed an original synthetic route towards the formation of polymetallic sulfido clusters combining lanthanide ions and biorelevant tetrathiomolybdate and tetrathiotungstate. These assemblies can readily bind nitrate and can further be electrodeposited onto Gas Diffusion Electrodes (GDE) to provide a homogenous deposit LnxMySz@GDL (M = Mo, W). Electrocatalytic nitrate reduction of these materials will be here presented.
Thanks to ETH Zurich for funding via an ETH research grant (ETH-44 19-1).
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