| Summary: | This paper aimed to investigate the structural and chemical changes of Ag-natrolite (Ag<sub>16</sub>Al<sub>16</sub>Si<sub>24</sub>O<sub>80</sub>·16H<sub>2</sub>O, Ag-NAT) in the presence of different pressure transmitting mediums (PTMs), such as N<sub>2</sub>, O<sub>2</sub> and CH<sub>4</sub>, up to ~8 GPa and 250 °C using in situ synchrotron X-ray powder diffraction and Rietveld refinement. Pressure-induced insertion occurs in two stages in the case of N<sub>2</sub> and O<sub>2</sub> runs, as opposed to the CH<sub>4</sub> run. First changes of the unit cell volume in N<sub>2</sub>, O<sub>2</sub> and CH<sub>4</sub> runs are observed at 0.88(5) GPa, 1.05(5) GPa and 1.84(5) GPa with increase of 5.7(1)%, 5.5(1)% and 5.7(1)%, respectively. Subsequent volume changes of Ag-natrolite in the presence of N<sub>2</sub> and O<sub>2</sub> appear at 2.15(5) GPa and 5.24(5) GPa with a volume increase of 0.8(1)% and a decrease of 3.0(1)%, respectively. The bulk moduli of the Ag-NAT change from 42(1) to 49(7), from 38(1) to 227(1) and from 49(3) to 79(2) in the case of N<sub>2</sub>, O<sub>2</sub> and CH<sub>4</sub> runs, respectively, revealing that the Ag-NAT becomes more incompressible after each insertion of PTM molecules. The shape of the channel window of the Ag-NAT changes from elliptical to more circular after the uptake of N<sub>2</sub>, O<sub>2</sub> and CH<sub>4</sub>. Overall, the experimental results of Ag-NAT from our previous data and this work establish that the onset pressure exponentially increases with the molecular size. The unit cell volumes of the expanded (or contracted) phases of the Ag-NAT have a linear relationship and limit to maximally expand and contract upon pressure-induced insertion.
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