Strong Swelling and Symmetrization in Siliceous Zeolites due to Hydrogen Insertion at High Pressure

Author:

Santoro Mario12ORCID,Rouquette Jérôme3ORCID,Fabbiani Marco3ORCID,di Renzo Francesco3ORCID,Coasne Benoît45ORCID,Dong Weiwei67,Glazyrin Konstantin6ORCID,Haines Julien3ORCID

Affiliation:

1. Istituto Nazionale di Ottica CNR-INO 50019 Sesto Fiorentino Italy

2. European Laboratory for Non Linear Spectroscopy (LENS) 50019 Sesto Fiorentino Italy

3. ICGM CNRS Université de Montpellier ENSCM 34293 Montpellier France

4. Université Grenoble Alpes CNRS, LIPhy 38000 Grenoble France

5. Institut Laue Langevin F-38042 Grenoble France

6. Deutsches Elektronen-Synchrotron DESY Notkestr. 85 22607 Hamburg Germany

7. Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 People's Republic of China

Abstract

AbstractHydrogen and helium saturate the 1D pore systems of the high‐silica (Si/Al>30) zeolites Theta‐One (TON), and Mobile‐Twelve (MTW) at high pressure based on x‐ray diffraction, Raman spectroscopy and Monte Carlo simulations. In TON, a strong 22 % volume increase occurs above 5 GPa with a transition from the collapsed P21 to a symmetrical, swelled Cmc21 form linked to an increase in H2 content from 12 H2/unit cell in the pores to 35 H2/unit cell in the pores and in the framework of the material. No transition and continuous collapse of TON is observed in helium indicating that the mechanism of H2 insertion is distinct from other fluids. The insertion of hydrogen in the larger pores of MTW results in a strong 11 % volume increase at 4.3 GPa with partial symmetrization followed by a second volume increase of 4.5 % at 7.5 GPa, corresponding to increases in hydrogen content from 43 to 67 and then to 93 H2/unit cell. Flexible 1D siliceous zeolites have a very high H2 capacity (1.5 and 1.7 H2/SiO2 unit for TON and MTW, respectively) due to H2 insertion in the pores and the framework, in contrast to other atoms and molecules, thereby providing a mechanism for strong swelling.

Funder

Deutsches Elektronen-Synchrotron

Agence Nationale de la Recherche

Région Auvergne-Rhône-Alpes

Publisher

Wiley

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