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66 CHAPTER4. RESULTSANDDISCUSSION (a) The O-covered RuO2 overlayer model (b) The O-covered TiO2 overlayer model electrode. electrode. Figure 4.15: The two model electrodes studied in Karlsson et al. [16]. Green balls are Ru, grey balls are Ti and red balls are O. face should be close to that optimal for ClER activity and selectivity. On the other hand, the RuO2-covered TiO2 surface should have electrocatalytic properties very similar to those of pure RuO2. By preparing such model electrodes and performing electrolysis experiments in chloride-containing electrolyte, it should be possible to compare the selectivity for ClER that the two model electrodes exhibit. We pre- dict that the ClER selectivity of the monolayer TiO2 on RuO2 electrode should be higher than that of the monolayer RuO2 on TiO2 electrode, and that both electrodes should be active. This same theoretical prediction was also made independently by Exner et al. [112] at almost the same time. 4.3 Semiclassical modeling of rutile oxides There is now a large literature indicating the value of theoretical modeling based on DFT. DFT is now a mainstream tool for materials science and catalysis. However, the computational cost of DFT calculations still makes some studies, specifically on the mesoscale, prohibitive. One such problem, that is expensive to tackle on the DFT level, is the study of the segregation of Ru and Ti in DSA. As has been in- dicated in previous sections[16, 17], the local structure of a mixed oxide electrode coating decides the electrocatalytic properties of the electrode. If the local struc- ture is to be controlled, tools to model the changes in local structure over time, both during preparation of the electrode and during use, are required. DSA coatings are made up by nanoscale particles of typically tens of nanometers size[37], so the model needs to be able to simulate particles of such size. A RuO2 particle with aPDF Image | Studies of Electrode Processes in Industrial Electrosynthesis
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