Spinodal decomposition of chemically fueled polymer solutions

Area of Science:

• Polymer chemistry
• Materials science
• Chemical engineering

Background:

• Out-of-equilibrium phase transitions are crucial for biological organization.
• Dissipative self-assembly uses chemical reaction networks (CRNs) to create transient structures.
• Limited research exists on the phase-separation process in chemically fueled systems.

Purpose of the Study:

• Investigate chemically fueled spinodal decomposition in poly(norbornene dicarboxylic acid) (PNDAc) solutions.
• Analyze the molecular-level CRN and the macroscopic phase separation process.
• Develop a model for predictive design of fueled polymer systems.

Main Methods:

• Studied the spinodal decomposition of PNDAc solutions driven by a cyclic CRN.
• Examined the morphology, kinetics, and mechanism of domain formation and growth.
• Developed a kinetic/thermodynamic hybrid model.

Main Results:

• Characterized the morphology of domains formed during chemically fueled spinodal decomposition.
• Quantified the kinetics and elucidated the mechanism of domain growth.
• The hybrid model successfully rationalized the system's dependence on fuel concentration and pH.

Conclusions:

• Chemically fueled spinodal decomposition offers a route to control transient polymer structures.
• The developed hybrid model provides a framework for predicting and designing fueled polymer systems.
• This work opens avenues for creating advanced functional materials through controlled dissipative self-assembly.