An NAD(P)H-Dependent Artificial Transfer Hydrogenase for Multienzymatic Cascades

作者:Okamoto Yasunori; Kohler Valentin; Ward Thomas R
来源:Journal of the American Chemical Society, 2016, 138(18): 5781-5784.
DOI:10.1021/jacs.6b02470

摘要

Enzymes typically depend on either NAD-(P)H or FADH(2) as hydride source for reduction purposes. In contrast, organometallic catalysts most often rely on isopropanol or formate to generate the reactive hydride moiety. Here we show that incorporation of a Cp*Ir cofactor possessing a biotin moiety and 4,7-dihydroxy-1,10-phenanthroline into streptavidin yields an NAD (P)H-dependent artificial transfer hydrogenase (ATHase). This ATHase (0.1 mol%) catalyzes imine reduction with 1 mM NADPH (2 mol%), which can be concurrently regenerated by a glucose dehydrogenase (GDH) using only 1.2 equiv of glucose. A four-enzyme cascade consisting of the ATHase, the GDH, a monoamine oxidase, and a catalase leads to the production of enantiopure amines.

  • 出版日期2016-5-11