Novel hydrogen clathrate hydrate

TL;DR

This paper reports the discovery of a new hydrogen clathrate hydrate with a disordered ice II-like structure, synthesized at high pressure and temperature, expanding understanding of hydrogen hydrate phases.

Contribution

It introduces a novel hydrogen clathrate hydrate with a disordered ice II structure, characterized by experimental and theoretical methods, differing from known ordered phases.

Findings

New hydrogen hydrate synthesized at 1.2 GPa and 298 K

Disordered hydrogen phase distinct from known ordered clathrates

Structural characterization confirms ice II-like oxygen lattice

Abstract

We report a new hydrogen clathrate hydrate synthesized at 1.2 GPa and 298 K documented by single-crystal X-ray diffraction, Raman spectroscopy, and first-principles calculations. The oxygen sublattice of the new clathrate hydrate matches that of ice II, while hydrogen molecules are in the ring cavities, which results in the trigonal R3c or R-3c space group (proton ordered or disordered, respectively) and the composition of (H2O)6H2. Raman spectroscopy and theoretical calculations reveal a hydrogen disordered nature of the new phase C1', distinct from the well-known ordered C1 clathrate, to which this new structure transforms upon compression and/or cooling. This new clathrate phase can be viewed as a realization of a disordered ice II, unobserved before, in contrast to all other ordered ice structures.