期刊
MICROPOROUS AND MESOPOROUS MATERIALS
卷 208, 期 -, 页码 21-29出版社
ELSEVIER
DOI: 10.1016/j.micromeso.2015.01.016
关键词
Metal-organic frameworks; Zirconium; UiO-67; Phosphoester; Hydrolysis
类别
资金
- FEDER (Fundo Europeu de Desenvolvimento Regional) through COMPETE (Programa Operacional Factores de Competitividade)
- FCT (Fundacao para a Ciencia e a Tecnologia) [FCOMP-01-0124-FEDER-037271, PEst-C/CTM/LA0011/2013, FCOMP-01-0124-FEDER-029779, PTDC/QEQ-SUP/1906/2012, BPD/UI89/4864/2013]
- Centro de Quimica Estrutural [PEst-OE/QUI/UI0100/2013]
- POCI (Programa Operacional Ciencia e Inovacao) [REDE/1517/RMN/2005]
- FCT
- Fundação para a Ciência e a Tecnologia [PTDC/QEQ-SUP/1906/2012, RECI/QEQ-QIN/0189/2012, PEst-OE/QUI/UI0100/2013] Funding Source: FCT
The Zr-IV-based metal-organic framework (MOF) UiO-67 has been examined as a promoter of the hydrolysis of phosphoester bonds by using sodium para-nitrophenylphosphate (pNPP) as a model substrate. The reactions were followed by H-1 NMR spectroscopy and performed under mild conditions using 2-100 mol% of the MOF relative to pNPP. All of the systems studied promoted the hydrolysis of pNPP to give para-nitrophenol (pNPh) and inorganic phosphate. A reaction half-life of ca. 30 min was achieved using 17 mol% of UiO-67 at 55 degrees C and 30 mol% at ambient temperature; >= 98% removal of pNPP was reached within 1 h for both reaction temperatures. H-1 NMR spectra of the reaction solutions, together with powder X-ray diffraction, FT-IR spectroscopy and solid-state NMR data for the recovered MOF, revealed that (i) pNPP was encapsulated and then converted to pNPh within the cavities of UiO-67, (ii) both pNPh and inorganic phosphate were retained in the solid promoter, and (iii) the MOF suffered partial structural breakdown into the components Zr6O4(OH)(4) and 4,4'-biphenyldicarboxylate, with partial release of the latter into solution. These structural changes eventually compromized the recyclability of the promoter, although the material could be recovered and reused in a second cycle without loss of activity. (C) 2015 Elsevier Inc. All rights reserved.
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