Atomistic Approach toward Selective Photocatalytic Oxidation of a Mustard-Gas Simulant: A Case Study with Heavy-Chalcogen-Containing PCN-57 Analogues.

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ACS applied materials & interfaces, ISSN: 1944-8252, Vol: 9, Issue: 23, Page: 19535-19540

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Goswami, Subhadip, Miller, Claire E, Logsdon, Jenna L, Buru, Cassandra T, Wu, Yi-Lin, Bowman, David N, Islamoglu, Timur, Asiri, Abdullah M, Cramer, Christopher J, Wasielewski, Michael R, Hupp, Joseph T, Farha, Omar K Show More Hide
American Chemical Society (ACS)
Materials Science
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Here we describe the synthesis of two Zr-based benzothiadiazole- and benzoselenadiazole-containing metal-organic frameworks (MOFs) for the selective photocatalytic oxidation of the mustard gas simulant, 2-chloroethyl ethyl sulfide (CEES). The photophysical properties of the linkers and MOFs are characterized by steady-state absorption and emission, time-resolved emission, and ultrafast transient absorption spectroscopy. The benzoselenadiazole-containing MOF shows superior catalytic activity compared to that containing benzothiadiazole with a half-life of 3.5 min for CEES oxidation to nontoxic 2-chloroethyl ethyl sulfoxide (CEESO). Transient absorption spectroscopy performed on the benzoselenadiazole linker reveals the presence of a triplet excited state, which decays with a lifetime of 9.4 μs, resulting in the generation of singlet oxygen for photocatalysis. This study demonstrates the effect of heavy chalcogen substitution within a porous framework for the modulation of photocatalytic activity.

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