- Physical Review Journals
All JournalsPhysics Magazine

Physical Review E

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Enhanced water evaporation via coupled capillary transport and gelation in confined nanocrystal systems

Zengbin Wang1, Dan Xu1,2, Qun Song1, Siyuan Liu1, Xintong Meng1, Shaohuang Chen1,3, Philipp Vana4,5, and Kai Zhang1,5,*

  • 1Sustainable Materials and Chemistry, Department of Wood Technology and Wood-based Composites, University of Göttingen, Büsgenweg 4, D-37077 Göttingen, Germany
  • 2Department of Material Chemistry, Graduate School of Engineering, Kyoto University, Kyoto 615–8510, Japan
  • 3State Key Laboratory of Chemical Engineering, Tianjin Key Laboratory of Membrane Science and Desalination Technology, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
  • 4Institute of Physical Chemistry, University of Göttingen, Tammannstr. 6, D-37077 Göttingen, Germany
  • 5Wöhler Research Institute for Sustainable Chemistry (WISCh), University of Göttingen, Tammannstr. 2, D-37077 Göttingen, Germany

  • *Contact author: kai.zhang@uni-goettingen.de
PDF

Phys. Rev. E 112, 045429 – Published 28 October, 2025

DOI: https://doi.org/10.1103/y5sn-g9vm

Abstract

Drying in confined systems is a critical process with broad implications, spanning applications from materials science to water management in microscale technologies. Nevertheless, the coupled dynamics of transport and gelation in confined drying of colloidal suspensions remains poorly understood. Here cellulose nanocrystals (CNCs) are employed as a model system to systematically investigate the temporal dynamics, kinetic behavior, and structural transformation of nanocrystal suspensions during capillary drying. We report a mechanism whereby CNC suspensions, upon exceeding a critical concentration (∼1 wt%), undergo a transition from a fluid-like state to a kinetically arrested gel state at the evaporation front. This transition is accompanied by pinning of the evaporation interface at the capillary opening and leads to the formation of a gel–film heterostructure, consisting of a CNC gel layer with a water concentration gradient and a thin surface film formed via interfacial slip. This heterostructure promotes directional water transport from the capillary interior to the interface and significantly enhances the effective evaporative area, thereby accelerating the overall drying process. These findings offer insights into confinement-driven drying behavior and establish a framework for regulating evaporation kinetics in colloidal systems.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (38)

  1. R. D. Deegan, O. Bakajin, T. F. Dupont, G. Huber, S. R. Nagel, and T. A. Witten, Capillary flow as the cause of ring stains from dried liquid drops, Nature (London) 389, 827 (1997).
  2. F. Clément and J. Leng, Evaporation of liquids and solutions in confined geometry, Langmuir 20 6538 (2004).
  3. U. Thiele, Patterned deposition at moving contact lines, Adv. Colloid Interface Sci. 206, 399 (2014).
  4. L. Daubersies and J.-B. Salmon, Evaporation of solutions and colloidal dispersions in confined droplets, Phys. Rev. E 84 031406 (2011).
  5. D. Brutin and V. Starov, Recent advances in droplet wetting and evaporation, Chem. Soc. Rev. 47 558 (2018).
  6. M. Cavallaro Jr., L. Botto, E. P. Lewandowski, M. Wang, and K. J. Stebe, Curvature-driven capillary migration and assembly of rod-like particles, Proc. Natl. Acad. Sci. USA 108 20923 (2011).
  7. S. K. Wilson and H.-M. D'Ambrosio, Evaporation of sessile droplets, Annu. Rev. Fluid Mech. 55 481 (2023).
  8. B. Pathak, S. Hatte, and S. Basu, Evaporation dynamics of mixed-nanocolloidal sessile droplets, Langmuir 33 14123 (2017).
  9. I. G. Hwang, J. Y. Kim, and B. M. Weon, Droplet evaporation with complexity of evaporation modes, Appl. Phys. Lett. 110, 031602 (2017).
  10. P. J. Yunker, T. Still, M. A. Lohr, and A. Yodh, Suppression of the coffee-ring effect by shape-dependent capillary interactions, Nature (London) 476 308 (2011).
  11. Y. Lin, E. Balizan, L. A. Lee, Z. Niu, and Q. Wang, Self-assembly of rodlike bio-nanoparticles in capillary tubes, Angew. Chem. Int. Ed. 49 868 (2010).
  12. R. D. Deegan, O. Bakajin, T. F. Dupont, G. Huber, S. R. Nagel, and T. A. Witten, Contact line deposits in an evaporating drop, Phys. Rev. E 62 756 (2000).
  13. P. Gurrala, S. Balusamy, S. Banerjee, and K. C. Sahu, A review on the evaporation dynamics of sessile drops of binary mixtures: Challenges and opportunities, Fluid Dyn. Mater. Process. 17 253 (2021).
  14. E. Bird and Z. Liang, Transport phenomena in the Knudsen layer near an evaporating surface, Phys. Rev. E 100 043108 (2019).
  15. G. Chen, On paradoxical phenomena during evaporation and condensation between two parallel plates, J. Chem. Phys. 159, 151101 (2023).
  16. R. Mondal and M. G. Basavaraj, Patterning of colloids into spirals via confined drying, Soft Matter 16 3753 (2020).
  17. R. A. Lopez de la Cruz, N. Schilder, X. Zhang, and D. Lohse, Phase separation of an evaporating ternary solution in a Hele-Shaw cell, Langmuir 37 10450 (2021).
  18. P. Bacchin, J. Leng, and J.-B. Salmon, Microfluidic evaporation, pervaporation, and osmosis: From passive pumping to solute concentration, Chem. Rev. 122 6938 (2021).
  19. V. Cherpak, V. Korolovych, R. Geryak, T. Turiv, D. Nepal, J. Kelly, T. Bunning, O. Lavrentovich, W. Heller, and V. Tsukruk, Robust chiral organization of cellulose nanocrystals in capillary confinement, Nano Lett. 18 6770 (2018).
  20. P. Liu, J. Wang, H. Qi, T. Koddenberg, D. Xu, S. Liu, and K. Zhang, Biomimetic confined self-assembly of chitin nanocrystals, Nano Today 43, 101420 (2022).
  21. W. Liu, J. Midya, M. Kappl, H.-J. Butt, and A. Nikoubashman, Segregation in drying binary colloidal droplets, ACS Nano 13 4972 (2019).
  22. T. Saito and A. Isogai, TEMPO-mediated oxidation of native cellulose. The effect of oxidation conditions on chemical and crystal structures of the water-insoluble fractions, Biomacromolecules 5, 1983 (2004).
  23. P. Liu, B. Pang, S. Dechert, X. C. Zhang, L. B. Andreas, S. Fischer, F. Meyer, and K. Zhang, Structure selectivity of alkaline periodate oxidation on lignocellulose for facile isolation of cellulose nanocrystals, Angew. Chem. Int. Ed. 59 3218 (2020).
  24. J. D. Goodrich and W. T. Winter, α-Chitin nanocrystals prepared from shrimp shells and their specific surface area measurement, Biomacromolecules 8 252 (2007).
  25. P. Liu, H. Liu, T. Schäfer, T. Gutmann, H. Gibhardt, H. Qi, L. Tian, X. C. Zhang, G. Buntkowsky, and K. Zhang, Unexpected selective alkaline periodate oxidation of chitin for the isolation of chitin nanocrystals, Green Chem. 23 745 (2021).
  26. See Supplemental Material at http://link.aps.org/supplemental/10.1103/y5sn-g9vm for further explanation of the simulation, additional experimental data, detailed derivations of theoretical results, and several illustrative figures.
  27. S. Mukherjee and H. Woods, X-ray and electron microscope studies of the degradation of cellulose by sulphuric acid, Biochim. Biophys. Acta 10, 499 (1953).
  28. Q. Song, Z. Wang, D. Xu, S. Liu, H. Liu, and K. Zhang, Self-assembly of polysaccharide nanocrystals: From aggregation in suspensions to optical materials, Prog. Polym. Sci. 148, 101768 (2024).
  29. E. Dussan, On the spreading of liquids on solid surfaces: Static and dynamic contact lines, Annu. Rev. Fluid Mech. 11 371 (1979).
  30. D. Xu, X. Meng, S. Liu, J. Poisson, P. Vana, and K. Zhang, Dehydration regulates structural reorganization of dynamic hydrogels, Nat. Commun. 15 6886 (2024).
  31. E. E. Ureña-Benavides, G. Ao, V. A. Davis, and C. L. Kitchens, Rheology and phase behavior of lyotropic cellulose nanocrystal suspensions, Macromolecules 44 8990 (2011).
  32. Y. Liu, J. Zhang, and P. Wu, Near-frictionless long-distance water transport in trees enabled by hierarchically helical molecular pumps, CCS Chem. 7, 484 (2025).
  33. M. Mashkour, T. Kimura, F. Kimura, M. Mashkour, and M. Tajvidi, Tunable self-assembly of cellulose nanowhiskers and polyvinyl alcohol chains induced by surface tension torque, Biomacromolecules 15 60 (2014).
  34. M. Mashkour, T. Kimura, M. Mashkour, F. Kimura, and M. Tajvidi, Printing birefringent figures by surface tension-directed self-assembly of a cellulose nanocrystal/polymer ink components, ACS Appl. Mater. Interfaces 11 1538 (2018).
  35. R. M. Parker, G. Guidetti, C. A. Williams, T. Zhao, A. Narkevicius, S. Vignolini, and B. Frka-Petesic, The self-assembly of cellulose nanocrystals: Hierarchical design of visual appearance, Adv. Mater. 30 1704477 (2018).
  36. P.-X. Wang, W. Y. Hamad, and M. J. MacLachlan, Structure and transformation of tactoids in cellulose nanocrystal suspensions, Nat. Commun. 7 11515 (2016).
  37. X. Zhou, F. Zhao, Y. Guo, B. Rosenberger, and G. Yu, Architecting highly hydratable polymer networks to tune the water state for solar water purification, Sci. Adv. 5 eaaw5484 (2019).
  38. K. I. Oh, K. Rajesh, J. F. Stanton, and C. R. Baiz, Quantifying hydrogen-bond populations in dimethyl sulfoxide/water mixtures, Angew. Chem. 129 11533 (2017).

Outline

Information

Phys. Rev. E 112, 045429– Published 28 October, 2025
  • Received 6 May 2025
  • Accepted 18 September 2025
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation