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1CO2 UTILIZATION PHOTOKAT and carbon monoxide (Fig. 35A), with smaller quantities of hydrogen and ethane also being produced. It is also noteworthy that under the standard reaction conditions (1.5 % CO2, 0.6 % H2O in helium, room temperature and a total pressure of 1.5 bar), none of the self-made (non-commercial) photo- catalysts exhibited activity greater than that observed with P25 for the pro- duction of carbon-containing products via the photocatalytic reduction of CO2. One commercial Au/TiO2 catalyst (AUROliteTM, STREM) did, however, exhibit higher activity for hydrogen generation, possibly via the preferential splitting of the water present in the gas phase. Pure P25 was therefore selected for the subsequent detailed mechanistic studies. Typically, three mechanisms are discussed in the literature. One in- volves CO as a key intermediate, another proceeds via formaldehyde and methanol, and the third via species that contain a C–C bond [11,12]. Of these three mechanisms, the first two could be ruled out under the reaction con- ditions employed in the current study. Titanium dioxide shows no activi- ty with respect to reaction with CO, so that even after 6 hours the initial concentration of CO was unchanged. Attempts to facilitate the formation of methane by depositing methanol, formaldehyde or formic acid onto the surface of the catalyst proved unsuccessful. None of these molecules show any appreciable electron affinity so that their oxidation or decomposition back to CO2 or CO will always be preferred to the reduction reaction forming methane. A mechanism involving C2 intermediates therefore appears much more probable than one involving the reduction of a C1 molecule to form methane [7,12]. This is why the photocatalytic conversion of molecules such as acetic acid or acetaldehyde, which could in principle be formed by coupling CO2 or CO with a methyl radical, leads to product distributions that are sim- ilar to those obtained from reducing CO2 to methane under standard con- ditions. [7]. If, however, the mechanism requires a C–C bond to be formed, it would be of interest to test approaches that have already been used in research in the field of conventional thermal heterogeneous catalysis, such as Fischer- Tropsch catalysis, in order to facilitate C–C bond formation. This might in- crease the yields of ethane and other longer chain hydrocarbons. Another potential research topic that has arisen from the project results concerns ac- celerating the release of the co-product oxygen. Oxygen was never detected as a reaction product, presumably because it remains bound by adsorption to the photocatalyst material. However, peroxides or superoxides that re- main in the catalyst material will ultimately lead to back reactions with the hydrocarbon products, thus reducing overall yields 92PDF Image | Chemical Processes and Use of CO2
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