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Structure Evolution of Chemically Degraded ZIF-8...

Publication Type
Journal
Journal Name
The Journal of Physical Chemistry C
Publication Date
Page Numbers
9736 to 9741
Volume
126
Issue
23

Exposure of the metal–organic zeolitic imidazolate framework-8 (ZIF-8) to humid SOx gas cleaves Zn–N bonds, leading to framework disorder and a corresponding decrease in pore accessibility. This work shows that framework disorder exhibits a critical behavior with respect to water concentration in the gas stream. While the quantity of sulfate adsorbed at Zn nodes is at or below the detection threshold for the X-ray pair distribution function technique, precluding direct observation of the adsorbate, powder diffraction reveals clear structural alterations. The onset of linker cleavage correlates to a large microstrain that diminishes as framework disorder increases. Energy-dispersive X-ray spectroscopy shows that the sulfur distribution throughout representative grains is uniform, implying the structure transformation is homogeneously nucleated and not dependent upon gas diffusion kinetics.