Most enzymatic redox reactions require cofactors. Because cofactors are expensive, cofactor regeneration is critical for practical redox enzyme processes. Rhodium-based organometallic catalysts (Rh complexes) were developed to regenerate biological cofactor molecules. However, when redox enzymes and Rh complexes are used together, mutual inactivation of both enzymes and Rh complexes happen. In order to overcome the mutual inactivation of Rh complex and enzyme, we investigated spatially controlled conjugation of Rh complex to a permissive site of a redox enzyme, in particular, mannitol dehydrogenase (MDH). When Rh complex was conjugated to a permissive site of MDH via a bioorthogonal reaction, the resulting dual function MDH-Rh complex maintained the catalytic activities as much as free Rh complex and MDH.

Artificial duel-functional enzyme constructed by combining an enzyme and an organometallic catalyst

2019 Spring National Meeting

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