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How Do Water Molecules Form a Hydrogen Bonding Network? Weiduo Zhu University of Science and Technology of China

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How Do Water Molecules Form a Hydrogen Bonding Network? Weiduo Zhu University of Science and Technology of China University of Nebraska - Lincoln DigitalCommons@University of Nebraska - Lincoln Xiao Cheng Zeng Publications Published Research - Department of Chemistry 2016 Two-dimensional interlocked pentagonal bilayer ice: how do water molecules form a hydrogen bonding network? Weiduo Zhu University of Science and Technology of China Wen- Hui Zhao University of Science and Technology of China Lu Wang University of Science and Technology of China Di Yin University of Science and Technology of China Min Jia University of Science and Technology of China See next page for additional authors Follow this and additional works at: http://digitalcommons.unl.edu/chemzeng Part of the Analytical Chemistry Commons, Materials Chemistry Commons, and the Physical Chemistry Commons Zhu, Weiduo; Zhao, Wen- Hui; Wang, Lu; Yin, Di; Jia, Min; Yang, Jinlong; Zeng, Xiao Cheng; and Yuan, Lan-Feng, "Two-dimensional interlocked pentagonal bilayer ice: how do water molecules form a hydrogen bonding network?" (2016). Xiao Cheng Zeng Publications. 148. http://digitalcommons.unl.edu/chemzeng/148 This Article is brought to you for free and open access by the Published Research - Department of Chemistry at DigitalCommons@University of Nebraska - Lincoln. It has been accepted for inclusion in Xiao Cheng Zeng Publications by an authorized administrator of DigitalCommons@University of Nebraska - Lincoln. Authors Weiduo Zhu, Wen- Hui Zhao, Lu Wang, Di Yin, Min Jia, Jinlong Yang, Xiao Cheng Zeng, and Lan-Feng Yuan This article is available at DigitalCommons@University of Nebraska - Lincoln: http://digitalcommons.unl.edu/chemzeng/148 Showcasing research from the laboratory of Dr Lan-Feng Yuan As featured in: and Prof. Xiao Cheng Zeng at University of Science and Technology of China Title: Two-dimensional interlocked pentagonal bilayer ice: how do water molecules form a hydrogen bonding network? An ideal H-bonding network of water should satisfy three requirements: four H-bonds per molecule, linear H-bonds, and tetrahedral configuration around each O atom. Under nanoscale confinement, some of them have to be unmet, and the selection of the specific requirement(s) leads to amazing multiplicity of structures. By sacrificing the linearity and retaining the tetrahedrality, a new 2D bilayer ice emerges, comprising interlocked pentagonal channels. See Xiao Cheng Zeng, Lan-Feng Yuan et al., Phys. Chem. Chem. Phys., 2016, 18, 14216. www.rsc.org/pccp Registered charity number: 207890 PCCP View Article Online PAPER View Journal | View Issue Two-dimensional interlocked pentagonal bilayer ice: how do water molecules form a hydrogen Cite this: Phys. Chem. Chem. Phys., 2016, 18,14216 bonding network? Weiduo Zhu,a Wen-Hui Zhao,a Lu Wang,a Di Yin,a Min Jia,a Jinlong Yang,a Xiao Cheng Zeng*ab and Lan-Feng Yuan*a 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 Creative Commons Attribution-NonCommercial 3.0 Unported Licence. 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 Received 7th December 2015, differences between the two bilayer structures due to the difference in the selection among the three Accepted 23rd March 2016 requirements. The IPBI sacrifices the linearity of hydrogen bonds to retain locally tetrahedral This article is licensed under a DOI: 10.1039/c5cp07524f 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 www.rsc.org/pccp understand the rich phase behaviors of nanoconfined water. Introduction hexagonal ice,16,17 bilayer hexagonal and rhombic ices,18–21 monolayer rhombic ices,22,23 trilayer ice,24 and trilayer hetero- Water is one of the most ubiquitous molecules on earth, and geneous fluid.25,26 remains to be a subject of intense interest. The phase diagram The multiplicity of the low-dimensional ice phases reflects the of bulk water is amazingly complicated: at least seventeen bulk extraordinary ability of water molecules to form diverse forms of crystalline ice phases have been found.1,2 Nanoscopic confinement hydrogen bonding networks. To understand this multiplicity of of water can disrupt and rearrange the hydrogen bonding ices in low-dimensions, we look into the selection among three networks, resulting in even more complex phase behavior.3–13 requirements for an ideal hydrogen bonding network of water: For instance, water confined in carbon nanotubes can form (1) four hydrogen bonds for every water molecule to maximize square, pentagonal, hexagonal, and octagonal single-walled ice the number of hydrogen bonds, (2) nearly linear hydrogen bonds nanotubes.4 In their simulations, Bai et al.14 observed high- to minimize the electrostatic repulsion between the donor and density nanoice exhibiting helical structures. Water confined acceptor O atoms, and (3) tetrahedral orientation for the four between two parallel plates can form many 2D ice polymorphs, hydrogen bonds around an O atom to match the four lobes of such as monolayer and bilayer square ice,15 distorted bilayer sp3 hybridization. For bulk ice, there exist many ways to fulfill the three requirements, leading to the multiplicity of bulk ice phases. Indeed, only in bulk ice, the hydrogen bonding network a Hefei National Laboratory for Physical Sciences at Microscale, can simultaneously satisfy the three requirements. The combination Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, China. E-mail: [email protected] of the three conditions means that the hydrogen bonding network b Department of Chemistry, University of Nebraska-Lincoln, Lincoln, NE 68588, is extended infinitely in all the three directions, therefore, under USA. E-mail: [email protected] nanoscale confinements, some of them must be unmet. This leads 14216 | Phys. Chem. Chem. Phys., 2016, 18, 14216--14221 This journal is © the Owner Societies 2016 View Article Online Paper PCCP to various possible selections on which condition to be sacrificed and which to be kept. For example, monolayer ices15,27 with in-plane hydrogen bonds sacrifice the tetrahedral orientation of the O atom to retain the linear hydrogen bonds, whereas another monolayer ice28 with out-of-plane O atoms sacrifices the linear hydrogen bonds to retain tetrahedrality. In addition to various basic motifs, different ways of compromise also lead to diverse forms of low-dimensional ice phases. In this work, we perform MD simulations for water confined between two hydrophobic parallel walls with the TIP5P water Fig. 1 A semi-quantitative D–T phase diagram of bilayer water confined between two hydrophobic walls. model. In particular, we find a new bilayer ice structure not reported in the literature, namely, the interlocked pentagonal bilayer ice (IPBI). The ‘‘coffin’’ structure in the literature,29 obtained based on the TIP4P water model, is similar to the IPBI in the top views, but exhibits fundamental structural differences due to different selection among the three requirements. The IPBI sacrifices linear hydrogen bonds to retain the tetrahedral orientation, while the coffin structure does the opposite. Simulation and analysis methods The simulation system is composed of 400 water molecules Creative Commons Attribution-NonCommercial 3.0 Unported Licence. confined between two smooth walls. The wall separation D (the difference between the heights of the two plates in the z direction) is set within the range of 0.8 nm to 1.0 nm. The water molecules interact with each other via the TIP5P pair potential30 and with the wall via the 9–3 Lennard-Jones (L-J) potential:31–35 s 9 s 3 UðDzÞ¼4e OW À OW (1) OW Dz Dz This article is licensed under a Here Dz is the distance from the oxygen atom of a water molecule to the wall, and the potential parameters are sOW =0.25nmand À1 19,36,37 eOW =1.25kJmol . Simulations were performed in the isothermal–isostress NPLT ensemble with periodic boundary conditions in the parallel (x and y) directions, where PL is the lateral pressure, set as 1 GPa. Temperature (T) and the lateral pressure are controlled using a Nose´–Hoover thermostat38,39 and Fig. 2 The potential energy U per water molecule as a function of T for various D values. a Parrinello–Rahman barostat,40 respectively. A cutoff of 1 nm is adopted for the L-J interactions, and the long-range electrostatic 41 interactions are treated by the slab-adapted Ewald sum method. For each D, the temperature T is lowered from 350 K to 230 K Depending on T and D, the simulations last for 10–100 ns, with a in a step of 10 K. First-order phase transitions between liquid MD step of 2 fs. and solid are indicated by abrupt changes of various properties. For instance, at T =250KandD = 0.9 nm, the potential energy U drops À1 Results and discussion by 3 kJ mol (Fig.
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