期刊
ACS APPLIED MATERIALS & INTERFACES
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.3c11858
关键词
ZIF-8; linker mixing; iodine adsorption; pore-structure; positron annihilation lifetime spectroscopy
This study proposes the incorporation of unsubstituted imidazole (Im) in zeolitic imidazolate framework-8 (ZIF-8) to greatly improve gas capture and gas separation performance. The incorporation of Im in ZIF-8 has been challenging due to the thermodynamic instability, but a delayed linker addition strategy at room temperature has successfully achieved up to 24.4 mol % Im linker incorporation. Im incorporation brings significant tuning to the pore architecture of ZIF-8, improving its crystal structure stability and iodine capture capability.
The incorporation of unsubstituted imidazole (Im) in zeolitic imidazolate framework-8 (ZIF-8) crystallized in sodalite topology is proposed to improve gas capture and gas separation performance drastically. However, the incorporation of unsubstituted Im in ZIF-8 has remained challenging due to the thermodynamic instability of zinc and Im bonding in sodalite topology. We have incorporated up to 24.4 (mol %) Im linker in highly crystalline ZIF-8 with similar morphology and sodalite topology using a delayed linker addition strategy at room temperature. Im incorporation brings significant tuning to the pore architecture of ZIF-8, as confirmed by positron annihilation lifetime spectroscopy. The modifications in the pore architecture are primarily due to linker defects produced in the frameworks during crystallization and the elimination of steric hindrance due to the absence of a methyl group on Im. The Im-incorporated ZIF-8 shows significant enhancement in iodine capture as well as higher crystal structure stability under iodine vapor exposure as compared to pristine ZIF-8. Through ortho-positronium interaction with the adsorbed molecular iodine in the pore network of the frameworks, it is confirmed that iodine is preferentially adsorbed at cavity and intercrystalline voids, whereas aperture sites remain unoccupied by iodine molecules.
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