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PHOTOKAT FUNDED PROJECTS Stable adsorption of CO2 was not detected on isolated titanates. It proved possible to increase the concentration of surface-adsorbed carbon dioxide by introducing isolated and agglomerated ZnO particles [6], though this had little effect on the activity of the catalysts with respect to methane forma- tion. If isolated titanate species are used as photocatalysts, the adsorption of CO2 on the surface of the material is not necessary and may even impede the reaction. The negative effect of strongly bound CO2, in this case in the form of car- bonates, was also demonstrated in studies of commercial titanium dioxide [7]. It was shown to be irrelevant whether carbonate formation was induced by surface modification or by sodium cations. Attempts to improve the methane yield through surface doping with other elements, such as divalent or tetravalent copper or tin, were also unsuccessful. The Cu-doped systems were, however, very active for hydrogen generation from aqueous methanol solutions [8]. Surface doping with Sn(II) accelerated the rate of selective hole transfer across the catalyst’s phase boundary into the surrounding medium [9], while grafting Sn(IV) on the surface of the TiO2 increased the rate of elec- tron transfer [10]. The latter stages of the project yielded significant insight into the reaction mechanism underlying the formation of methane on titanium dioxide [7]. An initial comparison of commercially available titanium dioxides showed that P25, which is a mixture of the two modifications anatase (80 %) and rutile (20 %), is the most active commercial material that also shows the lowest ac- tivity for the back reaction, i.e. decomposition of the hydrocarbon products. The main carbon-containing products generated with P25 were methane Fig. 34: A: Formation of methane and ethane on isolated titanate centres anchored on SBA-15 (T03) and commercial TS-1; B: Influence of photodeposited gold nanoparticles on the photocatalytic activity of titanate centres on SBA-15 in the formation of methane [3]; Reaction conditions: 1.5% CO2, 0.6% H2O in helium, irradiated with a 200-W HG(Xe) arc lamp. Measurement [h] AB Time 91 Yield [ppm] Yield CH4 [ppm]PDF Image | Chemical Processes and Use of CO2
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