Nitrate (NO3–) and perchlorate (ClO4–) are pervasive groundwater contaminants that are difficult to remove due to their high stability and resilience to reduction. Microorganisms express a group of molybdenum containing enzymes, nitrate reductase and perchlorate reductase, that can efficiently reduce nitrate and perchlorate. Motivated by the active site of Mo-containing metalloenzymes, we synthesized and characterized a dinuclear Mo(V) catalyst, Mo2O3(LBr)2(THF)2*2THF (1), where LBr = 5-bromo-2-hydroxybenzaldehyde thiosemicarbazone. In the presence of nitrate, 1 undergoes oxygen atom transfer (OAT) to yield MoVI(O)2(LBr)(MeOH) (2) and produce nitrite (NO2–). Complexes 1 and 2 were characterized by UV-vis, IR and NMR spectroscopies and X-ray crystallography. The addition of 0.25 equivalents of perchlorate to 1 allows perchlorate to undergo four OATs to yield 2 and Cl– in which the latter was detected and quantified by ion chromatography. With 5 mol% catalyst loading of 1 and triphenylphosphine added as an oxygen atom acceptor, a modest catalytic efficacy for the conversion of perchlorate to chloride was observed.

Catalytic reduction of perchlorate and nitrate by molybdenum catalyst

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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