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An ultralow-density porous ice with the largest internal cavity identified in the water phase diagram
Beijing Univ Chem Technol, Peoples R China; Univ Nebraska, NE 68588 USA.
Chinese Acad Sci, Peoples R China; Dalian Univ Technol, Peoples R China.
Univ Nebraska, NE 68588 USA; Univ Penn, PA 19104 USA; Univ Penn, PA 19104 USA.
Beijing Univ Chem Technol, Peoples R China.
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2019 (English)In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 116, no 26, p. 12684-12691Article in journal (Refereed) Published
Abstract [en]

The recent back-to-back findings of low-density porous ice XVI and XVII have rekindled the century-old field of the solid-state physics and chemistry of water. Experimentally, both ice XVI and XVII crystals can be produced by extracting guest atoms or molecules enclosed in the cavities of preformed ice clathrate hydrates. Herein, we examine more than 200 hypothetical low-density porous ices whose structures were generated according to a database of zeolite structures. Hitherto unreported porous EMT ice, named according to zeolite nomenclature, is identified to have an extremely low density of 0.5 g/cm(3) and the largest internal cavity (7.88 angstrom in average radius). The EMT ice can be viewed as dumbbell-shaped motifs in a hexagonal close-packed structure. Our first-principles computations and molecular dynamics simulations confirm that the EMT ice is stable under negative pressures and exhibits higher thermal stability than other ultralow-density ices. If all cavities are fully occupied by hydrogen molecules, the EMT ice hydrate can easily outperform the record hydrogen storage capacity of 5.3 wt % achieved with sII hydrogen hydrate. Most importantly, in the reconstructed temperature-pressure (T-P) phase diagram of water, the EMT ice is located at deeply negative pressure regions below ice XVI and at higher temperature regions next to FAU. Last, the phonon spectra of empty-sII, FAU, EMT, and other zeolite-like ice structures are computed by using the dispersion corrected vdW-DF2 functional. Compared with those of ice XI (0.93 g/cm(3)), both the bending and stretching vibrational modes of the EMT ice are blue-shifted due to their weaker hydrogen bonds.

Place, publisher, year, edition, pages
NATL ACAD SCIENCES , 2019. Vol. 116, no 26, p. 12684-12691
Keywords [en]
porous ice; ultralow density; EMT ice; reconstructed temperature-pressure phase diagram; record hydrogen storage capacity
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-158967DOI: 10.1073/pnas.1900739116ISI: 000472719100026PubMedID: 31182582OAI: oai:DiVA.org:liu-158967DiVA, id: diva2:1338142
Note

Funding Agencies|National Natural Science Foundation of China [21703006]; China Postdoctoral Science Foundation [2017M620582]; Swedish Research Council; US NSF [CHE-1665324]; University of Nebraska Holland Computing Center; University of Nebraska-Lincoln Nebraska Center for Energy Sciences Research

Available from: 2019-07-19 Created: 2019-07-19 Last updated: 2019-07-19

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