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Catalytic non-oxidative dehydrogenation (DH) of C3 – C4 alkanes is of increasing importance due to the growing demand for the corresponding olefins. Commercial catalysts with supported CrOx or Pt-Sn species have, however, shortcomings of being toxic or limited availability. Against this background, the present thesis was focused on the development of alternative DH catalysts on the basis of metal oxides with usually unchangeable metal oxidation state but with high ability for lattice oxygen removal.