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1CO2 UTILIZATION PHOTOKAT Fig. 33: Left: Schematic representation of the ultrapure gas-phase photoreactor with CF flange connections (1), quartz window (2), VCR connections (3), cooling jacket (4), sample holder (5) and cooling water feed line (6); Right: Photo of the reactor with valves and deflecting mirror for the 200-W Hg(Xe) arc lamp photocatalytic systems tested during the project. The activity data allowed the photocatalysts to be clearly distinguished from one another: Only the titanium dioxide-based materials exhibited any appreciable activity for the formation of methane from CO2. ZnO was far less active in this respect. Composites with gallium oxide, which were very active in photocatalytic water splitting, showed no activity for the formation of methane. Methanol was never detected as a product, even on titanium dioxide-based materials. However, other products were detected, including carbon monoxide, hydro- gen, ethane and traces of propane. The subsequent research work therefore focused on titanium dioxide sys- tems. It was shown that under ultrapure reaction conditions, a number of commercially available titanium dioxides and isolated tetrahedral titan- ate species in SiO2 functioned as active photocatalysts that were able to re- duce CO2 to methane [3]. In the first phase of the project, the isolated titan- ates were synthesised via a metalorganic anchoring mechanism (‘grafting’). It was later demonstrated, however, that the commercially available zeolite TS-1, which contains tetrahedrally coordinated titanium centres, can also function as an active photocatalyst for the reaction (Fig. 34A). This demon- strates that it is immaterial whether the titanates are anchored to the surface of the silicon dioxide or securely embedded within the SiO2 host lattice [4]. When gold nanoparticles were deposited onto TiOx/SBA-15, it was found that the methane yield almost doubled (Fig. 34B) [3]. However, under the con- ditions in which the gold nanoparticles were photodeposited, the previously isolated titanate centres became highly mobile and formed a TiOx-rich shell around the gold nanoparticles. It was demonstrated that this shell had a posi- tive effect on the electron transfer process involved in the photocatalysis [5]. 90PDF Image | Chemical Processes and Use of CO2
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