Abstract

Silica nanoparticles equipped with an artificial imine reductase display remarkable activity towards cyclic imine- and NAD(+) reduction. The method, based on immobilization and protection of streptavidin on silica nanoparticles, shields the biotinylated metal cofactor against deactivation yielding over 46 000 turnovers in pure samples and 4000 turnovers in crude cellular extracts.

Highlights

  • Silica nanoparticles equipped with an artificial imine reductase display remarkable activity towards cyclic imine- and NAD+ reduction

  • The method, based on immobilization and protection of streptavidin on silica nanoparticles, shields the biotinylated metal cofactor against deactivation yielding over 46 000 turnovers in pure samples and 4000 turnovers in crude cellular extracts

  • We have demonstrated the stability of enantioselectivity over time

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Summary

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D6-piano stool complexes have shown great potential for in vivo catalysis as they display promising stability in biological environments.[15] With the aim of improving its catalytic performance, we set out to shield an artificial transfer hydrogenase (ATHase) in a protective organosilica layer on silica nanoparticles (SNPs) and evaluate its catalytic performance towards the reduction of imines and the regeneration of NAD+.16. As shown previously with soluble ArMs, embedding the biotinylated pianostool iridium complex [Cp*Ir(biot-p-L)Cl] within various streptavidin mutants (Sav hereafter) allows to access either (R)- and (S)-salsolidine 2 (Fig. 1), depending on the Sav mutant (Table 1). In line with the performance of the soluble ArM, the immobilized [Cp*Ir(biot-p-L)Cl]ÁS112A-K121A Sav@prot-SNP yielded the best results, with TON of 12 885 and almost full conversion (entry 11). [Cp*Ir(biot-p-L)Cl]ÁS112A-K121A@prot-SNP [Cp*Ir(biot-p-L)Cl]ÁS112A-K121A@prot-SNP 1st recycling [Cp*Ir(biot-p-L)Cl]ÁS112A-K121A@prot-SNP 2nd recycling [Cp*Ir(biot-p-L)Cl]ÁS112A-K121A@prot-SNP 200 mM substratee [Cp*Ir(biot-p-L)Cl]ÁS112A-K121A Sav purified protein f

Native SNPs
Cellular debrisa
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