Dissipative operation of pH-responsive DNA-based nanodevices

Area of Science:

• Nanotechnology
• Biochemistry
• Chemical Engineering

Background:

• DNA-based nanodevices offer precise control over molecular processes.
• Dissipative operation requires continuous energy input to overcome equilibrium.
• Existing methods for powering nanodevices can be complex or limited.

Purpose of the Study:

• To demonstrate the utility of 2-(4-chlorophenyl)-2-cyanopropanoic acid (CPA) and nitroacetic acid (NAA) as chemical fuels.
• To utilize transient pH cycles generated by these fuels for dissipative nanodevice operation.
• To investigate the modulation and reversibility of nanodevice kinetics using these fuel acids.

Main Methods:

• Utilized CPA and NAA as chemical fuels in aqueous solutions.
• Monitored pH changes over time to characterize transient low-to-high pH cycles.
• Applied these pH cycles to control the operation of a DNA nanoswitch and a DNA-based receptor.
• Varied fuel acid concentrations to modulate system kinetics.

Main Results:

• CPA and NAA effectively drove dissipative operation of DNA nanodevices.
• Transient pH decrease followed by a slower increase was observed upon acid addition.
• Time-programmable open-close-open cycles of a DNA nanoswitch were achieved.
• A DNA-based receptor demonstrated controlled release-uptake of a DNA cargo strand.
• Nanodevice operation kinetics were modulated by fuel concentration.
• Both fuel acids exhibited efficient reversibility.

Conclusions:

• CPA and NAA are versatile and convenient chemical fuels for dissipative DNA nanodevices.
• The demonstrated pH-cycling mechanism provides a robust method for controlling nanodevice function.
• The reversibility and tunable kinetics of these fuels enhance their applicability in nanodevice engineering.