Water Confined in Nanocapillaries: Two-Dimensional Bilayer Squarelike Ice and Associated Solid-Liquid-Solid Transition

Weiduo Zhu, Yinbo Zhu, Lu Wang, Qiang Zhu, Wen Hui Zhao, Chongqin Zhu, Jaeil Bai, Jinlong Yang, Lan Feng Yuan, Hengan Wu, Xiao Cheng Zeng

Research output: Contribution to journalArticlepeer-review

23 Scopus citations


Despite recent experimental evidence of the two-dimensional (2D) square ice in graphene nanocapillaries, based on transmission electron microscopy (TEM) imaging, the AA-stacked bilayer square ice structure has not been observed in all previous classical molecular dynamics (MD) simulations nor found in recent unbiased first-principles structure searches. Herein, we report the MD simulations of 2D bilayer ice formation for water confined between two parallel hydrophobic walls (nanoslit). We find a bilayer ice whose simulated TEM imaging resembles that of bilayer squarelike ice. This bilayer ice also demonstrates dynamical stability in first-principles phonon computations. The realistic structure of this bilayer ice, however, consists of two hexagonal monolayers with the AB-stacking order, where the hexagonal rings are slightly elongated with two unequal inner angles, 107 and 146° (rather than 120°). The phase diagram of the nanoslit width versus temperature exhibits a solid-liquid-solid triple point, where the second solid phase is the well-known bilayer hexagonal ice (i.e., the bilayer ice I) with an AA-stacking order, which has been experimentally produced at ambient condition in a nanoslit of graphene and MoS2 sheet. Such a solid-liquid-solid triple point exhibits some resemblance to that shown in the pressure-temperature phase diagram for bulk ice I-water-ice III phases.

Original languageEnglish (US)
Pages (from-to)6704-6712
Number of pages9
JournalJournal of Physical Chemistry C
Issue number12
StatePublished - Mar 29 2018

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films


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