Open AccessHigh-Pressure Insertion of Dense H2 into a Model Zeolite
Author(s) -
Wan Xu,
Xiao-Di Liu,
Miriam Peña-Álvarez,
Haochuan Jiang,
Philip DalladaySimpson,
Benoît Coasne,
J. Haines,
Eugene Gregoryanz,
Mario Santoro
Publication year - 2021
Publication title -
journal of physical chemistry. c./journal of physical chemistry. c
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.401
H-Index - 289
eISSN - 1932-7455
pISSN - 1932-7447
DOI - 10.1021/acs.jpcc.1c02177
Subject(s) - zeolite , raman spectroscopy , intermolecular force , diffraction , synchrotron , materials science , monte carlo method , reverse monte carlo , crystallography , molecule , hydrogen , x ray crystallography , chemical physics , crystal structure , chemistry , catalysis , physics , organic chemistry , optics , neutron diffraction , statistics , mathematics
Our combined high-pressure synchrotron X-ray diffraction and Monte Carlo modeling studies show super-filling of the zeolite, and computational results suggest an occupancy by a maximum of nearly two inserted H 2 molecules per framework unit, which is about twice that observed in gas hydrates. Super-filling prevents amorphization of the host material up to at least 60 GPa, which is a record pressure for zeolites and also for any group IV element being in full 4-fold coordination, except for carbon. We find that the inserted H 2 forms an exotic topologically constrained glassy-like form, otherwise unattainable in pure hydrogen. Raman spectroscopy on confined H 2 shows that the microporosity of the zeolite is retained over the entire investigated pressure range (up to 80 GPa) and that intermolecular interactions share common aspects with bulk hydrogen, while they are also affected by the zeolite framework.