Assembling a single active pocket from enzyme and metal modules for simultaneously catalyzing oxidation-reduction...

Area of Science:

• Biochemistry
• Catalysis
• Materials Science

Background:

• Chemoenzymatic cascades integrate enzymatic and chemical catalysis for novel reactions.
• Diffusion resistance of intermediates limits cascade reaction efficiency.
• Integrating metal catalysts and enzymes can reduce diffusion resistance via proximity.

Purpose of the Study:

• To develop a single active pocket integrating enzymatic and dual metal-single-atom photocatalytic modules.
• To enable "one binding two reactions" catalysis, eliminating intermediate diffusion resistance.
• To achieve efficient oxidation-reduction cascades for directed detoxification of low-concentration mycotoxins.

Main Methods:

• Assembled enzymatic and dual metal-single-atom photocatalytic modules in a single active pocket.
• Utilized a hybrid active pocket for simultaneous transfer hydrogenation and oxidation catalysis under visible light.
• Demonstrated the elimination of intermediate diffusion and rebinding within the artificial active pocket.

Main Results:

• The enzyme-metal hybrid active pocket exhibited excellent catalytic activity.
• Achieved simultaneous transfer hydrogenation and oxidation reactions under visible light.
• Successfully demonstrated efficient oxidation-reduction cascades for mycotoxin detoxification.

Conclusions:

• Developed an innovative cascade process by integrating enzymatic and metal catalytic modules in a single active pocket.
• Eliminated diffusion resistance of reaction intermediates, enhancing catalytic efficiency.
• Established a powerful tool for editing enzyme active pockets with metal catalytic modules for targeted applications like mycotoxin detoxification.