Nitrogen-Neighbored Single-Cobalt Sites Enable Heterogeneous Oxidase-Type Catalysis

Area of Science:

• Catalysis
• Biomimetic Chemistry
• Materials Science

Background:

• Developing artificial enzymes that mimic natural oxidase activity is crucial for synthetic chemistry.
• Current biomimetic systems often struggle to achieve non-natural reactions or require harsh conditions.

Purpose of the Study:

• To create a robust, all-inorganic biomimetic catalytic system that mimics oxidase enzymes.
• To demonstrate its application in synthesizing valuable O-silylated compounds via aerobic oxidation.

Main Methods:

• Designed a biomimetic system with nitrogen-neighbored single-cobalt site/pyridinic-N site (Co-N4/Py-N) pairs.
• Utilized this system as an oxidase mimic for coupling oxygen reduction with chemical transformations.
• Applied the platform for the aerobic oxidation of hydrosilane under ambient conditions.

Main Results:

• Successfully demonstrated a cooperative oxidase mimic using the Co-N4/Py-N system.
• Achieved scalable synthesis of over 100 industrially and pharmaceutically relevant O-silylated compounds (silanols, borasiloxanes, silyl ethers).
• Showcased unprecedented aerobic oxidation of hydrosilane at ambient conditions.

Conclusions:

• The developed inorganic biomimetic system effectively mimics oxidase enzymes for synthetic applications.
• This platform offers a new route for synthesizing diverse O-silylated compounds and expands the scope of artificial enzymatic synthesis.
• The strategy provides insights into redox enzymes and opens avenues for novel biomimetic materials.