TY - JOUR
T1 - Two-dimensional interlocked pentagonal bilayer ice
T2 - How do water molecules form a hydrogen bonding network?
AU - Zhu, Weiduo
AU - Zhao, Wen Hui
AU - Wang, Lu
AU - Yin, Di
AU - Jia, Min
AU - Yang, Jinlong
AU - Zeng, Xiao Cheng
AU - Yuan, Lan Feng
N1 - Funding Information:
This work is supported by the National Natural Science Foundation of China (21503205, 21121003, 91021004, 20933006, and 51172223), by the Anhui Provincial Natural Science Foundation (1608085QB30), by CNPC and CAS (2015A-4812), by the National Key Basic Research Program (2011CB707305, 2011CB921404, and 2012CB922001), by Fundamental Research Funds for the Central Universities (WK2060140014 and WK2060190025), by CAS Strategic Priority Research Program (XDB01020300, XDB10030402), and by USTCSCC. XCZ is supported by grants from the University of Nebraska Center for Energy Sciences Research and a grant from USTC for (1000plan) Qianren-B summer research. WDZ, WHZ and XCZ are also supported by a grant (1401042004) from Bureau of Science & Technology of Anhui Province
Publisher Copyright:
© 2016 the Owner Societies.
PY - 2016
Y1 - 2016
N2 - The plethora of ice structures observed both in bulk and under nanoscale confinement reflects the extraordinary ability of water molecules to form diverse forms of hydrogen bonding networks. An ideal hydrogen bonding network of water should satisfy three requirements: (1) four hydrogen bonds connected with every water molecule, (2) nearly linear hydrogen bonds, and (3) tetrahedral configuration for the four hydrogen bonds around an O atom. However, under nanoscale confinement, some of the three requirements have to be unmet, and the selection of the specific requirement(s) leads to different types of hydrogen bonding structures. According to molecular dynamics (MD) simulations for water confined between two smooth hydrophobic walls, we obtain a phase diagram of three two-dimensional (2D) crystalline structures and a bilayer liquid. A new 2D bilayer ice is found and named the interlocked pentagonal bilayer ice (IPBI), because its side view comprises interlocked pentagonal channels. The basic motif in the top view of IPBI is a large hexagon composed of four small pentagons, resembling the top view of a previously reported "coffin" bilayer ice [Johnston, et al., J. Chem. Phys., 2010, 133, 154516]. First-principles optimizations suggest that both bilayer ices are stable. However, there are fundamental differences between the two bilayer structures due to the difference in the selection among the three requirements. The IPBI sacrifices the linearity of hydrogen bonds to retain locally tetrahedral configurations of the hydrogen bonds, whereas the coffin structure does the opposite. The tradeoff between the conditions of an ideal hydrogen bonding network can serve as a generic guidance to understand the rich phase behaviors of nanoconfined water.
AB - The plethora of ice structures observed both in bulk and under nanoscale confinement reflects the extraordinary ability of water molecules to form diverse forms of hydrogen bonding networks. An ideal hydrogen bonding network of water should satisfy three requirements: (1) four hydrogen bonds connected with every water molecule, (2) nearly linear hydrogen bonds, and (3) tetrahedral configuration for the four hydrogen bonds around an O atom. However, under nanoscale confinement, some of the three requirements have to be unmet, and the selection of the specific requirement(s) leads to different types of hydrogen bonding structures. According to molecular dynamics (MD) simulations for water confined between two smooth hydrophobic walls, we obtain a phase diagram of three two-dimensional (2D) crystalline structures and a bilayer liquid. A new 2D bilayer ice is found and named the interlocked pentagonal bilayer ice (IPBI), because its side view comprises interlocked pentagonal channels. The basic motif in the top view of IPBI is a large hexagon composed of four small pentagons, resembling the top view of a previously reported "coffin" bilayer ice [Johnston, et al., J. Chem. Phys., 2010, 133, 154516]. First-principles optimizations suggest that both bilayer ices are stable. However, there are fundamental differences between the two bilayer structures due to the difference in the selection among the three requirements. The IPBI sacrifices the linearity of hydrogen bonds to retain locally tetrahedral configurations of the hydrogen bonds, whereas the coffin structure does the opposite. The tradeoff between the conditions of an ideal hydrogen bonding network can serve as a generic guidance to understand the rich phase behaviors of nanoconfined water.
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U2 - 10.1039/c5cp07524f
DO - 10.1039/c5cp07524f
M3 - Article
C2 - 27063210
AN - SCOPUS:84971325339
SN - 1463-9076
VL - 18
SP - 14216
EP - 14221
JO - Physical Chemistry Chemical Physics
JF - Physical Chemistry Chemical Physics
IS - 21
ER -