Dissipative Constitutional Dynamic Networks for Tunable Transient Responses and Catalytic Functions

Area of Science:

• Supramolecular Chemistry
• Chemical Biology
• Systems Chemistry

Background:

• Living systems are controlled by dissipative, out-of-equilibrium processes.
• Understanding and mimicking these dynamic processes is crucial for synthetic biology.
• Constitutional dynamic networks (CDNs) offer a framework for creating adaptive chemical systems.

Purpose of the Study:

• To introduce nucleic acid-based dissipative constitutional dynamic networks (CDNs).
• To demonstrate tunable transient composition changes controlled by auxiliary fuel strands.
• To engineer emergent catalytic transformations within these dynamic networks.

Main Methods:

• Design and synthesis of nucleic acid constituents and fuel strands.
• Utilizing a nicking enzyme (Nt.BbvCI) for controlled network transitions.
• Kinetic simulations to predict and analyze network behavior under varying conditions.

Main Results:

• Demonstrated orthogonal dissipative transitions between different CDN states (X, Y, Z).
• Showcased programmed reconfiguration patterns of dissipative reaction cycles using fuel strands.
• Achieved emergent catalytic transformations through engineered nucleic acid tethers.

Conclusions:

• Nucleic acid-based CDNs provide a versatile platform for out-of-equilibrium systems.
• Tunable network dynamics can be achieved through external fuel strand input.
• Engineered CDNs can exhibit emergent catalytic functions, mimicking biological processes.