Programming Hydrogels with Complex Transient Behaviors via Autocatalytic Cascade Reactions.
ACS Appl Mater Interfaces
; 14(17): 20073-20082, 2022 May 04.
Article
em En
| MEDLINE
| ID: mdl-35439417
ABSTRACT
It is challenging to design complex synthetic life-like systems that can show both autoevolution and fuel-driven transient behaviors. Here, we report a new class of chemical reaction networks (CRNs) to construct life-like polymer hydrogels. The CRNs are constituted of autocatalytic cascade reactions and fuel-driven reaction networks. The reactions start with only two compounds, that is, thiol of 4-arm-PEG-SH and thiuram disulfides, and undergo thiol oxidation (k1), disulfide metathesis (k2), and thionate hydrolysis-coupling reactions (k3) subsequently, leading to a four-state autonomous transition of sol(I) â soft gel â sol(II) â stiff gel. Moreover, thiuram disulfides can be applied as a fuel to drive the repeated occurrence of metathesis and hydrolysis-coupling reactions, generating dissipative stiff gel â sol(II) â stiff gel cycles. Systematic kinetics studies reveal that the event and lifetime of every transient state could be delicately tailored-up by varying the thiuram disulfide concentration, pH of the system, and thiuram structures. Since the consecutive transient behaviors are precisely predictable, we envision the strategy's potential in guiding the molecular designs of autonomous and adaptive materials for many fields.
Texto completo:
1
Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
ACS Appl Mater Interfaces
Ano de publicação:
2022
Tipo de documento:
Article