Membraneless microdroplets generate thermodynamically distinct states of water under fully hydrated conditions
10 affiliations
- 1Biofunctional Catalyst Research Team
- 2RIKEN Center for Sustainable Resource Science (CSRS
- 3WPI Nano Life Science Institute (WPI-NanoLSI), Kanazawa University
- 4Materials Characterization Support Team
- 5RIKEN Center for Emergent Matter Science (CEMS
- 6Office of Research and Academia-Government-Community Collaboration, Hiroshima University, 1-3-2 Kagamiyama, Higashi-Hiroshima, Hiroshima, Japan
- 7Blue Marble Space, 600 1st Ave, Floor 1, Seattle, WA, USA, 98104
- 8Catalysis and Integrated Research Group
- 9Earth-Life Science Institute (ELSI
- 10Institute of Science Tokyo
Abstract
Water is indispensable for life, yet aqueous environments can thermodynamically disfavor dehydration-driven condensation reactions relevant to prebiotic polymer formation. Whether hydrated, dynamically reorganizing compartments can establish hydration thermodynamics distinct from the surrounding solution remains unclear. Here, we show that membraneless polyester microdroplets derived from prebiotically plausible α-hydroxy acids sustain spatially organized hydration environments during thermal structural reorganization. Combining high-speed scanning ion conductance microscopy, spatially resolved Raman spectroscopy and temperature-dependent wide-angle X-ray scattering, we resolve dynamic interfaces, spatial hydration gradients and reversible polymer organization. Crucially, Raman-derived average hydrogen-bond coordination within the droplets remains lower and markedly less temperature-dependent than in the corresponding aqueous solution. Van’t Hoff analysis of intact versus broken hydrogen bonds reveals attenuated apparent enthalpic and entropic contributions to redistribution. Together, these findings demonstrate that dynamically reconfiguring polymer-rich compartments can maintain distinct hydration thermodynamics during thermal perturbation, linking the physical chemistry of water with soft compartmentalization under hydrated conditions.
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BibTeX
@misc{chen2026membraneless,
title = {{Membraneless microdroplets generate thermodynamically distinct states of water under fully hydrated conditions}},
author = {Chen Chen and Shinji Watanabe and Linhao Sun and Kiyohiro Adachi and Priyanka Sharma and Tony Z. Jia and Aufandra Cakra Wardhana and Kosuke Dodo and Daisuke Hashizume and Ryuhei Nakamura},
howpublished = {ChemRxiv},
year = {2026},
month = oct,
doi = {10.26434/chemrxiv.15009972/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009972/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Membraneless microdroplets generate thermodynamically distinct states of water under fully hydrated conditions
AU - Chen Chen
AU - Shinji Watanabe
AU - Linhao Sun
AU - Kiyohiro Adachi
AU - Priyanka Sharma
AU - Tony Z. Jia
AU - Aufandra Cakra Wardhana
AU - Kosuke Dodo
AU - Daisuke Hashizume
AU - Ryuhei Nakamura
PY - 2026
DA - 2026/10/06
PB - ChemRxiv
DO - 10.26434/chemrxiv.15009972/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009972/v1
AB - Water is indispensable for life, yet aqueous environments can thermodynamically disfavor dehydration-driven condensation reactions relevant to prebiotic polymer formation. Whether hydrated, dynamically reorganizing compartments can establish hydration thermodynamics distinct from the surrounding solution remains unclear. Here, we show that membraneless polyester microdroplets derived from prebiotically plausible α-hydroxy acids sustain spatially organized hydration environments during thermal structural reorganization. Combining high-speed scanning ion conductance microscopy, spatially resolved Raman spectroscopy and temperature-dependent wide-angle X-ray scattering, we resolve dynamic interfaces, spatial hydration gradients and reversible polymer organization. Crucially, Raman-derived average hydrogen-bond coordination within the droplets remains lower and markedly less temperature-dependent than in the corresponding aqueous solution. Van’t Hoff analysis of intact versus broken hydrogen bonds reveals attenuated apparent enthalpic and entropic contributions to redistribution. Together, these findings demonstrate that dynamically reconfiguring polymer-rich compartments can maintain distinct hydration thermodynamics during thermal perturbation, linking the physical chemistry of water with soft compartmentalization under hydrated conditions.
ER -