Efforts toward the synthesis of a small molecule analogue of the active site of carbon monoxide dehydrogenase from Oligotropha carboxidovorans will be described.  The native active site contains a heterodimetallic [Mo-S-Cu] center, which is unique in biology and provides a synthetic challenge in biomimetic chemistry.  Our approach to this problem has involved a silane-mediated coupling reaction, which would tether a structurally relevant molybdenum-based fragment to an appropriate copper(I) moiety, thereby conserving the single-atom unsupported bridge [Mo-S-Cu] motif found in the native active site of the metalloenzyme.  New copper(I) silylthiolate complexes have been prepared and characterized, and the accompanying results from their respective coupling reactions will be discussed.  Several crystal structures of new reactants and products will be presented, along with general comments on the utility of silane-mediated coupling within the context of synthetic methodology.

Synthetic efforts toward a structural analog of molybdenum-dependent carbon monoxide dehydrogenase (CODH) via silane-mediated coupling reactions

245th National Meeting (2013)

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