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Operando Decoding Ion-Conductive Switch in Stimuli-Responsive Hydrogel by Nanodiamond-Based Quantum Sensing.
Ruqiang Dou1,2, Zan Li2, Guoli Zhu2
1Research Institute of Interdisciplinary Sciences & School of Materials Science and Engineering, Dongguan University of Technology, Dongguan, 523808, China.
Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
|September 23, 2024
Summary
Researchers developed thermal-responsive hydrogels as switches for energy storage. Nanodiamond quantum sensing revealed that microscopic phase separation physically blocks ion conduction at high temperatures, explaining the switch-off mechanism.
Area of Science:
- Materials Science
- Polymer Chemistry
- Nanotechnology
Background:
- Thermal-responsive hydrogels are promising for energy storage devices due to their ion-conductive switching capabilities.
- The precise molecular mechanism behind the on/off switching behavior of these hydrogels remains poorly understood.
Purpose of the Study:
- To investigate the molecular mechanism of ion conduction switching in thermal-responsive hydrogels.
- To elucidate the role of phase separation and nanoscale properties in hydrogel ion transport.
Main Methods:
- Synthesis of poly(N-isopropylacrylamide-co-acrylamide) hydrogel as a model system.
- In situ visualization of micro-scale phase separation and cross-linked mesh structure.
- Nanodiamond (ND) based quantum sensing to probe nanoscale viscosity, thermal conductivity, and ionic mobility.
Main Results:
- Micro-scale phase separation and a "chemically frozen" state of water molecules were observed during sol-gel transition.
- Nanoscale inhomogeneities in viscosity, thermal conductivity, and ionic mobility were detected using ND quantum sensing.
- Ionic mobility was found to be dependent on both temperature and polymer concentration.
Conclusions:
- Inhomogeneous phase separation at the microscale creates physical barriers that impede ion conduction pathways.
- This physical blocking mechanism provides a potential intrinsic explanation for the shutdown of ion migration in ionic hydrogels at elevated temperatures.

