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Zinc‐Substituted Polyoxotungstate@amino‐MIL‐101(Al) – An Efficient Catalyst for the Sustainable Desulfurization of Model and Real Diesels

2016; Wiley; Volume: 2016; Issue: 32 Linguagem: Inglês

10.1002/ejic.201600442

1099-0682

Diana Julião, Ana C. Gomes, Martyn Pillinger, Rita Valença, Jorge C. Ribeiro, Baltazar de Castro, Isabel S. Gonçalves, Luís Cunha‐Silva, Salete S. Balula,

Catalysis and Hydrodesulfurization Studies

The zinc‐substituted polyoxotungstate [PW 11 Zn(H 2 O)O 39 ] 5– (PW 11 Zn) has been encapsulated within the aluminium(III) 2‐aminoterephthalate NH 2 ‐MIL‐101(Al) metal–organic framework (MOF) either directly through a one‐pot microwave‐assisted synthesis or by an impregnation method. The resultant composite materials were characterized by elemental analysis, powder X‐ray diffraction, FTIR spectroscopy, and 31 P magic‐angle spinning (MAS) NMR spectroscopy. The desulfurization of a model diesel containing three refractory organosulfur compounds (1‐benzothiophene, dibenzothiophene, and 4,6‐dimethyldibenzothiophene) was studied with the ionic liquid 1‐butyl‐3‐methylimidazolium hexafluorophosphate as an extractant, the PW 11 Zn@MOF composites as sulfoxidation catalysts, and aqueous H 2 O 2 as an oxidant. The composite obtained by direct synthesis was the most efficient catalyst and led to almost complete desulfurization of the model diesel under mild conditions. Moreover, the solid catalyst could be recovered readily and recycled without significant loss of desulfurization performance. The application of this system to the treatment of a real diesel sample provided a very good sulfur removal of 83 % when combined with liquid–liquid extraction.