Nanostructured catalysts for the development of the hydrogen economy
|Advisor:||Kleitz, Freddy; Kaliaguine, S.|
|Abstract:||Catalysis plays an essential role in many industrial applications such as petrochemical and biochemical industries, as well as in the production of polymers and in environmental protection. Design and fabrication of efficient catalysts in a cost-effective way is an important milestone to address a number of unresolved issues in the new generation of chemical and energy conversion technologies. The objective of the studies in this thesis is the development of facile synthetic routes to prepare efficient catalysts based on non-noble metals, and elucidate fundamental aspects regarding the relationship between structure/composition and catalytic performance, in particular in the case of processes related to production and storage of hydrogen fuel. At first, a series of nanostructured porous mixed metal oxides (Cu/CeO2, CuFe/CeO2, CuCo/CeO2, CuFe2O4, NiFe2O4) have been synthesized via an improved nanocasting method. The porous structure of the nanocast products was tailored by tuning the mesostructure of the mesoporous silica phases used as templates. The obtained Cu/CeO2 materials with controlled composition and porous structure were then tested in preferential oxidation of CO in a hydrogen stream to achieve high purity hydrogen fuel. The synthesized catalysts exhibit high activity and selectivity in selective oxidation of CO to CO2. Regarding hydrogen storage, we reported a cost-effective synthetic way towards bi-component CuO-NiO catalyst showing excellent catalytic performance, which is comparable to noble metal catalysts, in the hydrogen generation from ammonia-borane. Moreover, we demonstrate that the interaction between Cu and Ni species is essential in accelerating hydrogen evolution of ammonia borane. The catalytic activity of the obtained catalyst investigated in this reaction is strongly influenced by the nature of the metal precursors, the composition and the thermal treatment temperature employed for the catalyst preparation. Finally, silica- and carbon-supported Cu-Ni nanocatalysts, with tunable composition and metal particle size, were synthesized by simple incipient wetness method. The carbon supported catalysts are stable, highly active and selective in both ammonia-borane hydrolysis and the decomposition of hydrous hydrazine for hydrogen evolution. We showed that optimal catalysts can be achieved through manipulation of bimetallic effect, metal-support interaction, and adequate metal particle size.|
|Document Type:||Thèse de doctorat|
|Open Access Date:||24 April 2018|
|Collection:||Thèses et mémoires|
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