期刊
JOURNAL OF CATALYSIS
卷 284, 期 2, 页码 194-206出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2011.07.008
关键词
Direct benzene oxidation; Fe/ZSM-5; Reaction mechanism; DFT calculations; Binuclear sites; N2O dissociation; Phenolate
资金
- Programme for Strategic Scientific Alliances between China and Netherlands [2008DFB50130]
- National Natural Science Foundation of China [20921092]
The stability of isolated extraframework Fe2+ ions in ZSM-5 zeolite and their reactivity in the benzene to phenol oxidation were studied by periodic OFT calculations. Mononuclear iron(II) cations can only be stabilized at very specific exchange sites of ZSM-5 zeolite. Accordingly, iron will be predominantly present as oxygenated/hydroxylated mono- and binuclear iron complexes in Fe/ZSM-5. The reactivity of isolated Fe2+. does not depend on the local coordination environment around iron, whereas the steric constraints imposed by the zeolite lattice are important for the overall catalytic reactivity. [FeO](+), [HOFe(mu-O)FeOH](2+), [Fe(mu-O)(2)Fe](2+), [Fe(mu-O)Fe](2+). extraframework complexes are also potential sites for benzene activation. The reaction is however not catalytic in these cases because the vacant active site cannot be regenerated. The presence of basic extraframework O ligands in these complexes favors phenol dissociation resulting in the formation of stable grafted phenolate species, and ultimately, to the deactivation of the oxygenated iron complexes. (C) 2011 Elsevier Inc. All rights reserved.
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