De novo synthesis of Cr-embedded MOF-199 and derived CuCr2O4/CuO porous composites for enhanced phenol hydroxylation
Date Issued
2016
Date
2016
Author(s)
Huang, Yu-Yuan
Abstract
The purpose of this study is to synthesize porous copper chromite/copper oxide (CuCr2O4/CuO) composites by a de novo synthesis of Cr-doped metal organic framework (MOF) as effective catalysts for phenol hydroxylation with enhanced selectivity. To desgin and synthesize a bimetallic solid catalyst, MOF-199 with copper source was chosen as the support for incorporating active species (i.e. Cr) through a de novo synthesis route, i.e. chromium ions were encapsulated into MOF-199 simultaneously upon the formation of the MOF-199 framework. The obtained Cr-MOF-199 samples were further calcined to convert into CuCr2O4/CuO composites that were characterized with XRD, SEM, TEM, and nitrogen sorption. The results showed that chromium ions were successfully embedded in the structure of MOF-199 uniformly, and the morphology of Cr-MOF-199 was changed from octahedral to cubic when chromium content was increased. The obtained porous CuCr2O4/CuO composites were further applied in phenol hydroxylation, and the results showed a high yield of 40% for diphenols (including hydroquinone and catechol) in optimized reaction conditions. It is worth of noting that the ratio of catechol/hydroquinone was enhanced from 1.3 to 1.8 with the existence of our synthesized CuCr2O4/CuO composites. The enhanced selectivity of catechol in phenol hydroxylation catalyzed by our newly synthesized CuCr2O4/CuO composites would provide a new application of MOF-derived catalysts.
Subjects
de novo synthesis
metal organic frameworks
copper oxide
copper chromite
phenol hydroxylation
MOF-derived composites
Type
thesis
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