Oleksenko L. Сatalytic activity in CO and H2 oxidation and phisico-chemical properties of d-metalcontaining loaded systems

Українська версія

Thesis for the degree of Doctor of Science (DSc)

State registration number

0509U000047

Applicant for

Specialization

  • 02.00.04 - Фізична хімія

19-01-2009

Specialized Academic Board

Д 26.001.03

Taras Shevchenko National University of Kyiv

Essay

. The loaded oxide and zeolite Co, Cu, Mn, Co-Pd, Cu-Pd, Mn-Pd-systems with various metal content in CO oxidation have been investigated. By DТА, XRD аnd ТPR it was shown that acti-vity of Со, Cu, Mn-catalysts with high metal content is defined with thermal stability of precursors and conditions of formation of catalyst resulting in various dispersity and extent of interaction of active phases with carriers. The activity of Со, Mn and Cu-systems with low metal content are сaused by distribution of ions, character of their interaction with support and ability to take part in redox transformations. The presence in surface layer of coorditative-unsaturated metal ions surrounded with extraframework oxygen in clusters with high reducible ability of ions and ability to adsorb CO in weakbonded form promotes high activity of 1,2%Co-, 3%Mn, 1,8%Cu-ZSM-5. High activity of bimetalcontaining systems in comparison with monometallic is caused with formation of additional centers. High active lowtemperature catalystsof CO аnd H2 oxidation at the base of heterogenized complexes of Pt and Pd than supported catalysts were obtained. Сomplexes -АPK and NAN'PTU with Pt and Pd possessed high activity only after partial ligand destruction while acetylacetonates does not decomposed. Kinetics reguliarities and mechanism of CO oxidation at Со, Сu, Co-Pd- and Сu-Pd/ZSM-5 were studied; on the heterogenized metal complexes the mechanism of Н2 and СО oxidation reations has been studied; it was shown that the experimental data agree with Eley - Rideal mechanism.

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