Enzyme-Compatible Core-Shell Nanoreactor for in Situ H₂ -Driven NAD(P)H Regeneration.

Area of Science:

• Catalysis
• Biotechnology
• Materials Science

Background:

• Efficient regeneration of nicotinamide adenine dinucleotide phosphate (NAD(P)H) is crucial for extracellular bioreduction applications.
• Existing NAD(P)H regeneration systems often lack compatibility with cascade enzymatic reduction processes.

Purpose of the Study:

• To develop an efficient and compatible artificial NAD(P)H regeneration catalytic system.
• To integrate a metal nanoparticle and metal complex into a core-shell nanoreactor for hydrogen-driven NAD(P)H regeneration.

Main Methods:

• Immobilization of a rhodium (Rh) complex onto a Ni/TiO2 surface using a bipyridine-containing 3D porous organic polymer (POP).
• Fabrication of a core-shell nanoreactor integrating metal nanoparticles (NPs) and a metal complex.
• Coupling the nanoreactor with aldehyde ketone reductase (AKR) for chemoenzymatic reduction.

Main Results:

• The integrated catalyst exhibited enhanced activity and selectivity in NAD(P)H regeneration compared to individual components.
• Activated hydrogen species spillover from metal NPs to the Rh complex significantly improved catalytic performance.
• The POP's size-sieving effect prevented enzyme-catalyst interaction, enabling successful chemoenzymatic reduction of acetophenone.

Conclusions:

• The developed core-shell nanoreactor provides an efficient strategy for hydrogen-driven NAD(P)H regeneration.
• This approach facilitates the successful coupling of artificial catalysts with enzymes for chemoenzymatic applications.
• The study offers a rational design strategy for multicomponent cooperative catalysis.