The thermally induced decarboxylation mechanism of a mixed-oxidation state carboxylate-based iron metal-organic framework.

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ID: 56523
2019
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Abstract
Investigations into a thermally generated decarboxylation mechanism for metal site activation and the generation of mesopores in a carboxylate iron-based MOF, PCN-250, have been conducted. PCN-250 exhibits an interesting oxidation state change during thermal treatment under inert atmospheres or vacuum conditions, transitioning from an Fe(iii)3 cluster to a Fe(ii)Fe(iii)2 cluster. To probe this redox event and discern a mechanism of activation, a combination of thermogravimetric analysis, gas sorption, scanning electron microscopy, 57Fe Mössbauer spectroscopy, gas chromatography-mass spectrometry, and X-ray diffraction studies were conducted. The results suggest that the iron-site activation occurs due to ligand decarboxylation above 200 °C. This is also consistent with the generation of a missing cluster mesoporous defect in the framework. The resulting mesoporous PCN-250 maintains high thermal stability, preserving crystallinity after multiple consecutive high-temperature regeneration cycles. Additionally, the thermally reduced PCN-250 shows improvements in the total uptake capacity of methane and CO2.
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drake2019thechemical Use this key to autocite in the manuscript while using SciMatic Manuscript Manager or Thesis Manager
Authors Drake, Hannah F;Day, Gregory S;Vali, Shaik Waseem;Xiao, Zhifeng;Banerjee, Sayan;Li, Jialuo;Joseph, Elizabeth A;Kuszynski, Jason E;Perry, Zachary T;Kirchon, Angelo;Ozdemir, Osman K;Lindahl, Paul A;Zhou, Hong-Cai;
Journal Chemical communications (Cambridge, England)
Year 2019
DOI
10.1039/c9cc04555d
URL
Keywords
oxidative stress morphology iron arabidospis thaliana cds qds esem/edx

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