Redox Chemical‐Fueled Dissipative Self‐Assembly of Active Materials

• Published in: ChemSystemsChem Vol. 2; no. 4
• Main Authors: Ogden, William A., Guan, Zhibin
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 01.07.2020
• Subjects: active materials; Chemical reactions; dissipative materials; fuelled self-assembly; hydrogels; redox chemistry; self-assembly
• ISSN: 2570-4206; 2570-4206
• DOI: 10.1002/syst.201900030

This work reports a new transient self‐assembly of active materials fueled solely by a mild redox reaction network. Fuel‐driven dissipative, out‐of‐equilibrium assemblies are common in living systems but are challenging to mimic synthetically. Synthetic dissipative assembly systems developed thus far often use relatively toxic fuels and harsh conditions. Herein we report a transient, out‐of‐equilibrium self‐assembly system based on a new chemical reaction network using redox reactions. We use a mild redox chemical reaction network to simultaneously create and destroy a disulfide‐based hydrogelator, leading to transient, dynamic behavior. By closely regulating the reaction kinetics and reagent composition, the macroscopic properties of the active materials are fine‐tuned. The current work represents an important step toward the development of active materials operating under mild conditions. Grow and learn: A new active material system was achieved by using a mild redox reaction network to fuel the dissipative self‐assembly of a disulfide‐based hydrogelator. The mild redox reactions simultaneously cause self‐assembled fibrils to grow and shrink, leading to transient, out‐of‐equilibrium dynamic behavior.