Harmonizing Enzyme-like Cofactors to Boost Nanozyme Catalysis

Area of Science:

• Materials Science
• Nanotechnology
• Catalysis

Background:

• Atomically dispersed metal sites in nanozymes mimic metallocofactors for catalysis.
• Existing nanozymes often neglect supporting cofactors, limiting electron transfer (ET) efficiency and catalytic performance.
• Optimizing nanozyme active sites requires considering synergistic effects of multiple cofactors.

Purpose of the Study:

• To engineer a nanozyme with atomically dispersed iron sites within a metal-organic framework (UiO-67).
• To incorporate multiple enzyme-like nanocofactors to enhance electron transfer and peroxidase-like catalysis.
• To demonstrate the nanozyme's application in sensitive detection of chlorpyrifos via immunoassay.

Main Methods:

• Fabrication of UiO-67 metal-organic framework with atomically dispersed iron sites.
• Integration of tailored enzyme-like nanocofactors, including linker-coupled iron sites, bare linkers, and zirconia nodes.
• Evaluation of peroxidase-like catalytic activity and electron transfer efficiency.
• Application in a sensitive immunoassay for chlorpyrifos detection.

Main Results:

• The engineered UiO-67 nanozyme exhibits synergistic catalysis driven by multiple nanocofactors.
• A 4.29-fold enhancement in catalytic activity was observed compared to isolated metal sites.
• The nanozyme demonstrated high sensitivity in detecting chlorpyrifos, showing promise for immunoassay applications.

Conclusions:

• Harmonizing multiple nanocofactors at the atomic and molecular scale is a viable strategy for designing high-performance nanozymes.
• The developed iron-based UiO-67 nanozyme offers enhanced peroxidase-like activity and sensitive analyte detection.
• This approach opens new avenues for creating advanced nanozymes by mimicking complex enzymatic active sites.