Development of an organic-inorganic route toward a better efficiency of NiMoO4 in propane oxidation

Farin, Benjamin
(2014)

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Authors
  • Farin, BenjaminUCLouvain
    author
Supervisors
Gaigneaux, Eric
 ;
Devillers, Michel
Abstract
This work is dedicated to the never-ending necessity to improve catalyst performances. More precisely, it aims at the synthesis of bulk NiMoO4 having properties that are usually difficult to meet. Therefore, our strategy is based on the valorization of a polyampholytic comb-like copolymer matrix (poly[N,N-diallyl-N-alkylamine-alt-(maleic acid)]) used as a template. This matrix displays a supramolecular organization thanks to hydrophobic interactions between its alkyl side chains. The as-prepared NiMoO4 are then tested in the propane ODH reaction to check if their properties lead to better catalytic performances. Firstly, hybrid precursors associating Ni & Mo ions and the copolymer are prepared by taking advantage of the copolymer charges. Their systematic characterization enables to clarify their organization, the ion – matrix interactions and the ion amount that the matrix can fix. Moreover, the charge state and the alkyl side chain length are two tunable parameters of the copolymer. Their impact on the synthesis and the organization of the hybrids is here also studied. Upon optimization of the calcination temperature, of the hybrid homogeneity and of the copolymer alkyl side chain length, mesoporous β-NiMoO4 are then prepared via calcination of the hybrids. This β-phase is the most selective in propene but is also metastable and requires hard calcination conditions. Although, the exothermic matrix burning enables to crystallize it under soft temperatures. More propene selective catalysts are so synthesized without sacrificing their porosity that originates from the initial matrix organization. Their catalytic activity is thus also preserved. In the end, our hybrid method yields more productive NiMoO4 than those made from classical methods.
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Farin, B. (2014). Development of an organic-inorganic route toward a better efficiency of NiMoO4 in propane oxidation. https://hdl.handle.net/2078.5/49730