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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 H2 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 H2 forms an exotic topologically constrained glassy-like form, otherwise unattainable in pure hydrogen. Raman spectroscopy on confined H2 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.
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