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. 2012 Aug 15;17(8):9835-41.
doi: 10.3390/molecules17089835.

Towards recyclable NAD(P)H regeneration catalysts

Miriam de Torres  1 , Jonas Dimroth, Isabel W C E Arends, Juliane Keilitz, Frank Hollmann
Affiliations

Towards recyclable NAD(P)H regeneration catalysts

Miriam de Torres et al. Molecules. .

Abstract

Rh(III)-TsDPEN, an immobilized analog of the well-known [Cp*Rh(bpy)(H(2)O)](2+) was evaluated as a heterogeneous, recyclable regeneration catalyst for reduced oxidoreductase cofactors [NAD(P)H]. Repeated use of this catalyst was established and the catalytic properties were initially investigated. Apparently, Rh(III)-TsDPEN is prone to severe diffusion limitations, necessitating further developments. Overall, a promising concept for chemoenzymatic redox catalysis is proposed, which may overcome some of the current limitations such as catalyst cost and incompatibility of Rh with some biocatalysts.

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Figures

Scheme 1
Scheme 1
Immobilized Cp*Rh complex (Rh(III)-TsDPEN) evaluated in this study; and its application to promote NAD(P)H-regeneration. Support: Surface-functionalized poly(ethylene) sinter chips [17].
Figure 1
Figure 1
Recycling experiments with Rh(III)-TsDPEN. Upper: time courses of the single experiments (1:formula image; 2:formula image; 3:formula image; 4:formula image; 5:formula image; 6:formula image; 7:formula image; 8:formula image; 9:formula image; 10:formula image); lower: initial rates. Conditions: 50 mg Rh(III)-TsDPEN (0.35 μmol), c(NAD+)0 = 0.25 mM, 50 mM phosphate buffer pH 7, T = 30 °C, c(NaHCO2) = 150 mM, 1,000 rpm; 100% corresponds to an NADH-generation rate of 0.21 mM·h−1.
Figure 2
Figure 2
Temperature-dependence of the NAD+-reduction. Conditions: 50 mg Rh(III)-TsDPEN (0.35 μmol), c(NAD+)0 = 0.25 mM, c(NaHCO2) = 150 mM, 1,000 rpm.
Figure 3
Figure 3
Dependence of Rh(III)-TsDPEN activity on c(NAD+)0, expressed as TOF(Rh). Conditions: 50 mg Rh(III)-TsDPEN (0.35 μmol), T = 30 °C, c(NaHCO2) = 150 mM, 1,000 rpm.
See this image and copyright information in PMC

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