Enzyme-Instructed Interfacial Jamming of Pillar[5]arenes for Macroscopic Signal Amplification

Area of Science:

• Supramolecular Chemistry
• Biochemical Engineering
• Materials Science

Background:

• Enzyme-instructed signal generation offers novel macroscopic control and detection of biochemical processes.
• Self-assembly at liquid-liquid interfaces is key for creating dynamic material properties.

Purpose of the Study:

• To explore pillar[5]arene (P[5]A) self-assembly and interfacial jamming for signal generation.
• To develop an enzyme-instructed system for amplifying and detecting alkaline phosphatase (ALP) activity.
• To investigate the use of macroscopic surface changes as a readout for biochemical detection.

Main Methods:

• Utilized copper-mediated "click" reactions for P[5]A self-assembly at oil-water interfaces.
• Investigated interfacial jamming dynamics by varying P[5]A and ascorbic acid (AA) concentrations.
• Implemented an enzyme-triggered "click" reaction using dephosphorylation of a dormant reductant by ALP for signal amplification.

Main Results:

• Achieved self-assembly and interfacial jamming of P[5]A derivatives, forming networks that alter droplet shapes.
• Demonstrated tunable surface coverage and jamming dynamics by controlling reactant concentrations.
• Successfully amplified ALP activity into observable macroscopic surface changes, with inhibition observed in the presence of heavy metals and chelators.

Conclusions:

• Pillar[5]arene self-assembly at liquid-liquid interfaces provides a versatile platform for enzyme-instructed signal generation.
• The developed system enables sensitive quantification of ALP activity through macroscopic readouts.
• This approach holds promise for biochemical sensing and materials science applications requiring signal amplification.