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Title: Structure of ice confined in silica nanopores

Abstract

Observed anomalous thermodynamic properties of confined water such as deviations in the melting point and freezing point motivate the determination of the structure of confined water as a function of pore size and temperature. Here, we investigate the dynamic evolution of the structure of confined ice in SBA-15 porous materials with pore diameters of 4 nm, 6 nm, and 8 nm at temperatures ranging from 183 K to 300 K using in operando Wide-Angle X-Ray Scattering (WAXS) measurements, X-Ray Partial Distribution Function (PDF) measurements, and classical Molecular Dynamics (MD) simulations. Formation of hexagonal ice structures is noted in all the three pore sizes. In silica nanopores with diameters of 4 nm, cubic ice formation is noted in addition to hexagonal ice. Longer lasting hydrogen bonds and longer residence times of the water molecules in the first coordination shell contribute to observed crystalline organization of ice in confinement. Self-diffusion coefficients of confined liquid water, predicted from classical MD simulations, are four orders of magnitude higher compared to ice formed in confinement. These experimental and simulation results provide comprehensive insights underlying the organization of confined water and ice in silica nanopores and the underlying physico-chemical interactions that contribute to the observed structures.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Cornell Univ., Ithaca, NY (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Univ. of Utah, Salt Lake City, UT (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1808583
Alternate Identifier(s):
OSTI ID: 1784798; OSTI ID: 1828845
Grant/Contract Number:  
SC0019285; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 23; Journal Issue: 22; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; water; ice; silica; pores; confinement; molecular dynamics; Wide Angle X-Ray Scattering (WAXS) measurements

Citation Formats

Mohammed, Sohaib, Asgar, Hassnain, Benmore, Chris J., and Gadikota, Greeshma. Structure of ice confined in silica nanopores. United States: N. p., 2021. Web. doi:10.1039/d1cp00686j.
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Mohammed, Sohaib, Asgar, Hassnain, Benmore, Chris J., & Gadikota, Greeshma. Structure of ice confined in silica nanopores. United States. https://doi.org/10.1039/d1cp00686j
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Mohammed, Sohaib, Asgar, Hassnain, Benmore, Chris J., and Gadikota, Greeshma. Mon . "Structure of ice confined in silica nanopores". United States. https://doi.org/10.1039/d1cp00686j. https://www.osti.gov/servlets/purl/1808583.
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@article{osti_1808583,
title = {Structure of ice confined in silica nanopores},
author = {Mohammed, Sohaib and Asgar, Hassnain and Benmore, Chris J. and Gadikota, Greeshma},
abstractNote = {Observed anomalous thermodynamic properties of confined water such as deviations in the melting point and freezing point motivate the determination of the structure of confined water as a function of pore size and temperature. Here, we investigate the dynamic evolution of the structure of confined ice in SBA-15 porous materials with pore diameters of 4 nm, 6 nm, and 8 nm at temperatures ranging from 183 K to 300 K using in operando Wide-Angle X-Ray Scattering (WAXS) measurements, X-Ray Partial Distribution Function (PDF) measurements, and classical Molecular Dynamics (MD) simulations. Formation of hexagonal ice structures is noted in all the three pore sizes. In silica nanopores with diameters of 4 nm, cubic ice formation is noted in addition to hexagonal ice. Longer lasting hydrogen bonds and longer residence times of the water molecules in the first coordination shell contribute to observed crystalline organization of ice in confinement. Self-diffusion coefficients of confined liquid water, predicted from classical MD simulations, are four orders of magnitude higher compared to ice formed in confinement. These experimental and simulation results provide comprehensive insights underlying the organization of confined water and ice in silica nanopores and the underlying physico-chemical interactions that contribute to the observed structures.},
doi = {10.1039/d1cp00686j},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 22,
volume = 23,
place = {United States},
year = {Mon May 17 00:00:00 EDT 2021},
month = {Mon May 17 00:00:00 EDT 2021}
}
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