ISIS Neutron and Muon Source Data Journal

Deep Structural Investigation of Hysteresis-Free Hydrogels Enabled by Liquid?Liquid Phase Separation

Abstract: Zwitterionic hydrogels prepared via liquid liquid phase separation (LLPS) exhibit a remarkable, near-ideal elasticity, with >99% reversibility and <1% hysteresis over repeated high-strain cycles. The nanoscale architecture responsible for this fatigue-free elasticity remains unknown. Here, we propose to resolve this structure using small-angle neutron scattering (SANS). We will conduct a systematic SANS study to track the time-dependent evolution (0 24 h) of the LLPS-derived nanostructure and quantify its transformation upon the addition of crosslinkers and photoinitiators, and through the final photocuring step. Crucially, contrast variation (H O/D O) will decouple polymer and solvent scattering, enabling precise in-situ determination of key structural parameters: domain sizes, correlation lengths, and solvent organization. By correlating these nanostructural readouts with macroscopic mechanical testing (stretchability, cyclic hysteresis), we will establish the definitive structure-property relationship governing this unusual elasticity. This knowledge will provide the first rational design principles for engineering fatigue-free elasticity into next-generation soft materials. Preliminary data confirm the SANS profile's high sensitivity to both LLPS duration and chemical additives, validating the feasibility of this investigation and motivating a focused 72-hour campaign to resolve the governing nanostructural motifs.

Principal Investigator: Mr Yiming Ma
Experimenter: Mr Yue Shao
Experimenter: Professor Molly Stevens
Local Contact: Dr James Doutch
Experimenter: Mr Zile Zhuang
Experimenter: Mr Li Ma

DOI: 10.5286/ISIS.E.RB2610205

ISIS Experiment Number: RB2610205

Publisher: STFC ISIS Neutron and Muon Source

Data format: RAW/Nexus
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Data Citation

The recommended format for citing this dataset in a research publication is as:
[author], [date], [title], [publisher], [doi]

For Example:
Mr Yiming Ma et al; (2026): Deep Structural Investigation of Hysteresis-Free Hydrogels Enabled by Liquid?Liquid Phase Separation, STFC ISIS Neutron and Muon Source, https://doi.org/10.5286/ISIS.E.RB2610205

Data is released under the CC-BY-4.0 license.