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This study introduces novel chemo-bio catalysts for efficient, enantioselective hydrogenation using H2-driven NADH regeneration. These catalysts combine metal/carbon materials with enzymes for cleaner chemical synthesis.

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Area of Science:

  • Catalysis
  • Biochemistry
  • Green Chemistry

Background:

  • Heterogeneous biocatalytic hydrogenation offers a sustainable route for enantioselective reductions.
  • Enzyme-catalyzed reactions often require efficient cofactor regeneration systems, such as nicotinamide adenine dinucleotide (NADH).
  • Hydrogen gas (H2) is a clean reductant, but its direct application in biocatalysis needs effective activation and cofactor recycling.

Purpose of the Study:

  • To develop and characterize novel chemo-bio catalysts for direct H2-driven NAD+ reduction.
  • To investigate the use of carbon-supported metal (metal/C) catalysts for H2 oxidation and electron transfer to adsorbed enzymes.
  • To demonstrate the application of these integrated systems for enantioselective ketone reductions using alcohol dehydrogenase.

Main Methods:

  • Commercial metal/C catalysts were evaluated for direct H2-driven NAD+ reduction.
  • Selected metal/C catalysts were coupled with enzymes on conductive carbon supports for H2 oxidation and NAD+ reduction.
  • Characterization of metal/C catalysts and carbon supports to identify key properties influencing activity.
  • Optimized chemo-bio catalysts were used with alcohol dehydrogenase for enantioselective ketone reductions.

Main Results:

  • Chemo-bio catalysts demonstrated improved activity and selectivity for generating bioactive NADH under ambient conditions.
  • High cofactor turnover numbers and enzyme activities were achieved (e.g., 441 h-1 for Pd and 2347 h-1 for NAD+ reductase).
  • Enantioselective ketone reductions proceeded with >99% enantiomeric excess (ee).

Conclusions:

  • A novel strategy for combining chemo- and biocatalysis on carbon supports was successfully demonstrated.
  • This integrated approach provides an efficient and sustainable method for producing bioactive NADH.
  • The developed chemo-bio catalysts are effective for enantioselective hydrogenation reactions, offering a greener alternative to traditional methods.