HYDROGENASE ACTIVE SITES: A NEW PARADIGM FOR NATURAL PRODUCT-INSPIRED SYNTHESIS BASED ON ORGANOMETALLIC CHEMISTRY

Abstract

The scientific career of F.G.A. Stone witnessed the birth of transition metal organic chemistry and contributed greatly through an amazing period of development. The maturation and acceptance of this new field depended on the accumulated syntheses and careful characterization of compounds that spanned the transition metal series, setting “in Stone” the precedents, principles, and tenets of structure and bonding of species containing a metal-carbon bond.^{[ 1 ]} These well-described observations from Stone's laboratory permitted predictions that guided applications to homogeneous catalysis from the organic chemist's bench to the industrial plant processes. This new organometallic chemistry ultimately changed our lives. Nevertheless, there was “old” organometallic chemistry, well developed in nature from billions of years of evolution. It was just waiting to be discovered when the chemistry in our Schlenk flasks, signals from our spectra, and structures from our crystal tubes were sufficiently understood.

Keywords:

• hydrogenase
• organoiron
• small molecule models
• synthetic analogues

Abbreviations:

• eas
• enzyme active site
• H₂ase
• hydrogenase

ACKNOWLEDGEMENT

We acknowledge financial support from the National Science Foundation (CHE-0910679 to MYD, and CHE-0541587) and the R.A. Welch Foundation (A-0924).