Formation of porous ice frameworks at room temperatureShow others and affiliations
2021 (English)In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 118, no 31, article id e2104442118Article in journal (Refereed) Published
Abstract [en]
Bulk crystalline ices with ultralow densities have been demonstrated to be thermodynamically metastable at negative pressures. However, the direct formation of these bulk porous ices from liquid water at negative pressures is extremely challenging. Inspired by approaches toward porous media based on host-guest chemistry, such as metal-organic frameworks and covalent organic frameworks, we herein demonstrate via molecular dynamics simulations that a class of ultralow-density porous ices with upright channels can be formed spontaneously from liquid water at 300 K with the assistance of carbon nanotube arrays. We refer to these porous ice polymorphs as water oxygen-vertex frameworks (WOFs). Notably, our simulations revealed that the liquid-WOF phase transition is first-order and occurs at room temperature. All the WOFs exhibited the unique structural feature that they can be regarded as assemblies of nanoribbons of hexagonal bilayer ice (2D ice I) at their armchair or zigzag edges. Based on density functional theory calculations, a comprehensive phase diagram of the WOFs was constructed considering both the thermodynamic and thermal stabilities of the porous ices at negative pressures. Like other types of porous media, these WOFs may be applicable to gas storage, purification, and separation. Moreover, these biocompatible porous ice networks may be exploited as medicalrelated carriers.
Place, publisher, year, edition, pages
NATL ACAD SCIENCES , 2021. Vol. 118, no 31, article id e2104442118
Keywords [en]
porous; ice; crystalline
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-178516DOI: 10.1073/pnas.2104442118ISI: 000685040600006PubMedID: 34326263OAI: oai:DiVA.org:liu-178516DiVA, id: diva2:1587010
Note
Funding Agencies|National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [21703006, 11772144]; Fundamental Research Funds for the Central UniversitiesFundamental Research Funds for the Central Universities; Sun Yat-sen University [2021qntd13]; Swedish Research CouncilSwedish Research CouncilEuropean Commission; University of Nebraska Holland Computing Center
2021-08-232021-08-232021-08-23