High-Pressure Insertion of Dense H-2 into a Model Zeolite

Year: 2021

Authors: Xu W., Liu X., Pena-Alvarez M., Jiang H., Dalladay-Simpson P., Coasne B., Haines J., Gregoryanz E., Santoro M.

Autors Affiliation: Chinese Acad Sci, Inst Solid State Phys, Key Lab Mat Phys, HFIPS, Hefei 230031, Peoples R China; Univ Sci & Technol China, Hefei 230026, Peoples R China; Univ Edinburgh, Ctr Sci Extreme Condit, Edinburgh EH9 3FD, Midlothian, Scotland; Univ Edinburgh, Sch Phys & Astron, Edinburgh EH9 3FD, Midlothian, Scotland;Ctr High Pressure Sci & Technol Adv Res, Shanghai 201203, Peoples R China; Univ Grenoble Alpes, LIPhy, CNRS, F-38000 Grenoble, France; Univ Montpellier, ENSCM, CNRS, ICGM, F-34095 Montpellier, France; Ist Nazl Ott CNR INO and European Lab Non Linear Spect LENS, I-50019 Sesto Fiorentino, Italy

Abstract: 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.


Volume: 125 (13)      Pages from: 7511  to: 7517

More Information: The research was supported by the Chinese Academy of Sciences President´s International Fellowship Initiative Fund (2019VMA0027), the National Natural Science Foundation of China (grant nos. 11874361, 51672279, 11774354, and 51727806), the CAS Innovation Grant (CXJJ-19-B08), the Science Challenge Project (no. TZ2016001), and the CASHIPS Director´s Fund (grant no. YZJJ201705). We also acknowledge the PRIN project ZAPPING, number 2015HK93L7, granted by the Italian Ministry of Education, Universities and Research, MIUR. MPA acknowledges the support of the European Research Council (ERC) Grant Hecate Ref. no. 695527. Some of the computations presented in this paper were performed using the Froggy platform of the GRICAD infrastructure (https://gricad.univ-grenoble-alpes.fr), which is supported by the Rhone-Alpes region (GRANT CPER07 13 CIRA) and the Equip@Meso project (reference ANR-10-EQPX-29-01) of the programme Investissements d´Avenir supervised by the Agence Nationale pour la Recherche.
KeyWords: Crystals; Diffraction; Hydrogen; Molecules; Zeolites
DOI: 10.1021/acs.jpcc.1c02177

Citations: 5
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