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Synthesis and stability of xenon oxides Xe2O5 and Xe3O2 under pressure.

Accepted version
Peer-reviewed

Repository DOI


Type

Article

Change log

Authors

Dewaele, Agnès 
Worth, Nicholas 
Pickard, Chris J 
Needs, Richard J 
Pascarelli, Sakura 

Abstract

The noble gases are the most inert group of the periodic table, but their reactivity increases with pressure. Diamond-anvil-cell experiments and ab initio modelling have been used to investigate a possible direct reaction between xenon and oxygen at high pressures. We have now synthesized two oxides below 100 GPa (Xe2O5 under oxygen-rich conditions, and Xe3O2 under oxygen-poor conditions), which shows that xenon is more reactive under pressure than predicted previously. Xe2O5 was observed using X-ray diffraction methods, its structure identified through ab initio random structure searching and confirmed using X-ray absorption and Raman spectroscopies. The experiments confirm the recent prediction of Xe3O2 as a stable xenon oxide under high pressure. Xenon atoms adopt mixed oxidation states of 0 and +4 in Xe3O2 and +4 and +6 in Xe2O5. Xe3O2 and Xe2O5 form extended networks that incorporate oxygen-sharing XeO4 squares, and Xe2O5 additionally incorporates oxygen-sharing XeO5 pyramids. Other xenon oxides (XeO2, XeO3) are expected to form at higher pressures.

Description

Keywords

0306 Physical Chemistry (incl. Structural)

Journal Title

Nat Chem

Conference Name

Journal ISSN

1755-4330
1755-4349

Volume Title

8

Publisher

Springer Science and Business Media LLC
Sponsorship
Engineering and Physical Sciences Research Council (EP/J017639/1)
Engineering and Physical Sciences Research Council (EP/K014560/1)
The authors acknowledge the European Synchrotron Radiation Facility for provision of beamtime under proposals HS-4067 and HC-767. Financial support was provided by the Engineering and Physical Sciences Research Council (EPSRC) of the UK [EP/J017639/1]. Computational resources were provided by the High Performance Computing Service at the University of Cambridge and the Archer facility of the UK’s national high-performance computing service, for which access was obtained via the UKCP consortium [EP/K014560/1]. C.J.P. is supported by the Royal Society through a Royal Society Wolfson Research Merit Award. Nano-polycrystalline diamond anvils were prepared based on JSPS grants (No. 25220712 and No.15H05829) to T.I.