Reaction of H<sub>2</sub> with mitochondria-relevant metabolites using a multifunctional molecular catalyst.

Yoshioka, Shota; Nimura, Sota; Naruto, Masayuki; Saito, Susumu · Sci Adv · 2020

basic_science · Level V

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Abstract

The Krebs cycle is the fuel/energy source for cellular activity and therefore of paramount importance for oxygen-based life. The cycle occurs in the mitochondrial matrix, where it produces and transfers electrons to generate energy-rich NADH and FADH<sub>2</sub>, as well as C<sub>4</sub>-, C<sub>5</sub>-, and C<sub>6</sub>-polycarboxylic acids as energy-poor metabolites. These metabolites are biorenewable resources that represent potential sustainable carbon feedstocks, provided that carbon-hydrogen bonds are restored to these molecules. In the present study, these polycarboxylic acids and other mitochondria-relevant metabolites underwent dehydration (alcohol-to-olefin and/or dehydrative cyclization) and reduction (hydrogenation and hydrogenolysis) to diols or triols upon reaction with H<sub>2</sub>, catalyzed by sterically confined iridium-bipyridyl complexes. The investigation of these single-metal site catalysts provides valuable molecular insights into the development of molecular technologies for the reduction and dehydration of highly functionalized carbon resources.