Organophophorous Ester Degradation by Chromium(III) Terephthalate Metal–Organic Framework (MIL-101) Chelated to N,N-Dimethylaminopyridine and Related Aminopyridines

Autor:	Lev Bromberg, Sa Wang, Heidi Schreuder-Gibson, T. Alan Hatton
Rok vydání:	2013
Předmět:	Chemistry Inorganic chemistry chemistry.chemical_element Catalysis Hydrolysis Chromium chemistry.chemical_compound Nucleophile General Materials Science Chelation Metal-organic framework Lewis acids and bases Acetonitrile Nuclear chemistry
Zdroj:	ACS Applied Materials & Interfaces. 5:1269-1278
ISSN:	1944-8252 1944-8244
DOI:	10.1021/am302359b
Popis:	Porous materials based on chromium(III) terephthalate metal organic frameworks (MOF) MIL-101(Cr) and their complexes with dialkylaminopyridines (DAAP) were synthesized via a DAAP-MOF complexation, and tested for hydrolytic degradation of organophosphorous esters such as diethyl 4-nitrophenyl phosphate (paraoxon). Elemental analysis, TGA, XRD, FT-IR, TEM, SEM, and nitrogen adsorption measurements indicated that the DAAP units were incorporated into MIL-101 pores by complexation, keeping the parent framework intact. The DAAP-MOF enabled facile paraoxon hydrolysis in water/acetonitrile mixtures under ambient conditions (100% conversion after 24 h at pH 10). The MOF-DAAP complexes showed synergistic effects, being 7-fold and 47-fold more active than the parent MIL-101 or DAAP materials, respectively. The high hydrolysis reaction turnover was realized by simultaneous action of the Lewis acid Cr(III) center of the MOF as well as the electron-rich nucleophile, DAAP. This study demonstrates a simple and efficient method of generating catalytically active MOF materials for environmental detoxification as well as defensive applications.
Databáze:	OpenAIRE
Externí odkaz:	https://explore.openaire.eu/search/publication?articleId=doi_dedup___::1f3fbcd93c86ead3f465badb5c3877f2 https://doi.org/10.1021/am302359b Zobrazit plný text záznamu