Ice Regelation: Hydrogen-bond extraordinary recoverability and water quasisolid-phase-boundary dispersivity

Zhang, Xi; Huang, Yongli; Sun, Peng; Liu, Xinjuan; Ma, Zengsheng; Zhou, Yue; Zhou, Ji; Zheng, Weitao; Sun, Chang Q.

doi:10.1038/srep13655

Cited by 22 publications

(16 citation statements)

References 37 publications

(70 reference statements)

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“…Unlike other materials whose phonons were harden by external pressure, ice-VIII demonstrated the anomalous softening of the H-O vibration mode at frequency greater than 3000 cm −1 while stiffening of the O:H vibration mode at frequency lower than 400 cm −1 17. Ice melts under compression and freezes again when the pressure is relieved, evidencing extraordinary recoverability of O:H-O bond21. Hydrogen bond interaction potential, typical double-well potentials of the symmetrical22 and the asymmetrical23 forms, is still under debate.…”

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confidence: 89%

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Hydrogen-bond potential for ice VIII-X phase transition

Zhang

Chen

2016

Sci Rep

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Repulsive force between the O-H bonding electrons and the O:H nonbonding pair within hydrogen bond (O-H:O) is an often overlooked interaction which dictates the extraordinary recoverability and sensitivity of water and ice. Here, we present a potential model for this hidden force opposing ice compression of ice VIII-X phase transition based on the density functional theory (DFT) and neutron scattering observations. We consider the H-O bond covalent force, the O:H nonbond dispersion force, and the hidden force to approach equilibrium under compression. Due to the charge polarization within the O:H-O bond, the curvatures of the H-O bond and the O:H nonbond potentials show opposite sign before transition, resulting in the asymmetric relaxation of H-O and O:H (O:H contraction and H-O elongation) and the H+ proton centralization towards phase X. When cross the VIII-X phase boundary, both H-O and O:H contract slightly. The potential model reproduces the VIII-X phase transition as observed in experiment. Development of the potential model may provide a choice for further calculations of water anomalies.

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confidence: 89%

“…Based on our extensive investigation of water anomalies21343536, we proposed hidden force model for dynamics of the “O: H-O” bond under external pressures, as shown in Fig. 1a.…”

Section: Potential Model Proposedmentioning

confidence: 99%

Hydrogen-bond potential for ice VIII-X phase transition

Zhang

Chen

2016

Sci Rep

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“…However, compression disperses the boundaries inwardly, lowering the melting temperature and raising the freezing temperature, call Regelation [89]. (Reprinted with permission from [2,90,93]).…”

Section: From the F(1/d) Inmentioning

confidence: 99%

Supersolidity of undercoordinated and hydrating water

Sun

2018

Phys. Chem. Chem. Phys.

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Supersolid water, firstly defined in 2013 [J Phys Chem Letter 4: 2565; ibid 4: 3238] and intensively verified since then, refers to those water molecules being polarized by molecular undercoordination (often called confinement such as nanobubbles and droplets) or by salt hydration. This work shows that a combination of the STM/S, XPS, NEXFAS, SFG, DPS, ultrafast UPS, and ultrafast FTIR observations and quantum theory calculations confirmed the bond−electron−phonon correlation in the supersolid phase. The supersolidity is characterized by the shorter and stiffer H−O bond and longer and softer O:H nonbond, O 1s energy entrapment, hydrated electron polarization and the longer lifetime of photoelectrons and phonons. The supersolid phase is less dense, elastoviscous, mechanically and thermally more stable with the hydrophobic and frictionless surface. The O:H−O bond cooperative relaxation disperses outwardly the quasisolid phase boundary to raise the melting point and meanwhile lower the freezing temperature of the quasisolid phase -called supercooling and superheating. Highlight  Molecular undercoordination and ionic hydration effect the same on O:H−O relaxation  XPS O 1s and K-edge absorption energy shifts in proportional to the H−O bond energy  Electron hydration probes the site-and size-resolved bounding energy and the electron lifetime  DPS, SFG, and calculations confirm the site-resolved H−O contraction and thermal stability

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“…Faraday argued that the liquid layers remain on a surface but they froze solid when they were at the interface. He also used this mechanism to explain the observation of ice regelation-ice melts under compression and freezes again when the pressure is relieved [20].…”

Section: Quasiliquid Skin Notionmentioning

confidence: 99%

From ice superlubricity to quantum friction: Electronic repulsivity and phononic elasticity

Zhang

Huang

et al. 2015

Friction

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Superlubricity means non-sticky and frictionless when two bodies are set contacting motion. Although this occurrence has been extensively investigated since 1859 when Faraday firstly proposed a quasiliquid skin on ice, the mechanism behind the superlubricity remains uncertain. This report features a consistent understanding of the superlubricity pertaining to the slipperiness of ice, self-lubrication of dry solids, and aqueous lubricancy from the perspective of skin bond-electron-phonon adaptive relaxation. The presence of nonbonding electron polarization, atomic or molecular undercoordination, and solute ionic electrification of the hydrogen bond as an addition, ensures the superlubricity. Nonbond vibration creates soft phonons of high magnitude and low frequency with extraordinary adaptivity and recoverability of deformation. Molecular undercoordination shortens the covalent bond with local charge densification, which in turn polarizes the nonbonding electrons making them localized dipoles. The locally pinned dipoles provide force opposing contact, mimicking magnetic levitation and hovercraft. O:H−O bond electrification by aqueous ions has the same effect of molecular undercoordination but it is throughout the entire body of the lubricant. Such a Coulomb repulsivity due to the negatively charged skins and elastic adaptivity due to soft nonbonding phonons of one of the contacting objects not only lowers the effective contacting force but also prevents charge from being transited between the counterparts of the contact. Consistency between theory predictions and observations evidences the validity of the proposal of interface elastic Coulomb repulsion that serves as the rule for the superlubricity of ice, wet and dry frictions, which also reconciles the superhydrophobicity, superlubricity, and supersolidity at contacts.

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Ice Regelation: Hydrogen-bond extraordinary recoverability and water quasisolid-phase-boundary dispersivity

Cited by 22 publications

References 37 publications

Hydrogen-bond potential for ice VIII-X phase transition

Hydrogen-bond potential for ice VIII-X phase transition

Supersolidity of undercoordinated and hydrating water

From ice superlubricity to quantum friction: Electronic repulsivity and phononic elasticity

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