Hydrolytic and Peroxyhydrolytic Degradation of Nerve Agent Analogs with Low Molecular Weight Bimetallic Catalysts
Final rept. 1 Aug 2001-31 Dec 2004
MIAMI UNIV CORAL GABLES FL DEPT OF CHEMISTRY
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The proposed research focused on the detoxification of both G- and V-types nerve agents by chemical means. Two key objectives are i developing novel hetero-bimetallic FeZn TACN complexes that facilitate efficient hydrolysis of both organophosphate esters and G-agents, and ii synthesizing Mn2-complexes of TACN and probe their activities in catalyzing oxidative degradation of VX-simulants sulfides using either O2 or H2O2. Early on, we succeeded in the preparation of the tethered bis-TACN ligands. However, clean synthesis of hetero-bimetallic FeZn complexes remains a challenge. The effort during the later stage 2002-2004 was focused on the activation of H2O2 and tBuO2H for the oxygenation of organic sulfides, which is the key step in V-agent degradation. Proficiency of bimetallic Mn-TACN system was explored and the effect of co-catalysts was evaluated. It is also found that the mononuclear Mn-TACN system can activate tBuO2H and exhibits one of the highest TOFs turn-over frequency in the oxygenation of sulfides by tBuO2H. Also identified is an organic soluble polyoxometallate catalyst, Bu4N4GAMMA-SiW10O34H2O2, which displays both a remarkable 100 utility of H2O2 in catalytic sulfide oxygenation and chemical selectivity for sulfoxide formation. Several graduate and undergraduate students both female and underrepresented groups participated all phases of ARO funded research.
- Inorganic Chemistry
- Properties of Metals and Alloys