Mechanozyme: An Artificial Enzyme With a Mechanophore Framework

Area of Science:

• Biochemistry
• Molecular Biology
• Nanotechnology

Background:

• Natural enzymes exhibit conformational flexibility and marginal stability, leading to functional variations.
• Artificial enzymes, such as DNAzymes, are being developed to mimic or surpass natural enzyme capabilities.

Purpose of the Study:

• To investigate marginal stability in artificial DNAzymes.
• To explore mechanical modulation of DNAzyme catalytic activity.
• To establish a new class of enzymes termed 'mechanozymes'.

Main Methods:

• Utilized G-quadruplex (GQ)-hemin complexes to create artificial DNAzymes.
• Employed single-molecule fluorescent MT-HILO (Magnetic Tweezers coupled with Highly Inclined and Laminated Optical sheet) to measure activity under force.
• Applied ultrasonication to a large ensemble of DNAzymes.

Main Results:

• Demonstrated that DNAzymes made of GQ-hemin complexes exhibit marginal stability.
• Observed the highest peroxidase activity in DNAzymes when the GQ mechanophore was destabilized by external force.
• Showcased enhanced catalytic function in a large ensemble of DNAzymes via ultrasonication, weakening GQ structures.

Conclusions:

• Established marginal stability in artificial enzymes for the first time.
• Provided unprecedented mechanical modulation of catalytic activities in DNAzymes.
• Highlighted the potential of mechanozymes for catalysis in chemistry and biosciences.