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4.2. SELECTIVITY BETWEEN CL2 AND O2 63 ∆E(Oc ), 50% surface coverage ∆E(Oc ), 100% surface coverage Optimal ∆E(Oc ) ∆E(Oc ) on pure TiO2 ∆E(Oc ) on pure RuO2 5 4 3 2 1 1cus 1br 2a 2b 3a Ru position 3b 4a 4b Figure 4.12: The effect on the Oc adsorption energy at the CUS site of Ru-doped TiO2. The position of the Ru atom is varied. The system is either a 1x1 system (100% surface coverage) or a 1x2 system with adsorption of O only on one CUS site (50% surface coverage). The dashed lines for the adsorption energies on pure materials are from calculations on 1x1 surface systems. Figure reprinted from Karlsson et al. [16], with permission from Elsevier. als with higher concentrations of dopants near the active site. Furthermore, it is seen in the figure that while the doped TiO2 material is strongly affected by the Ru dopant, the RuO2 material is hardly affected at all. Some insight into the inherent stability of different dopant-Ti arrangements can be gained by comparing the total energies of the two arrangements in Figure 4.10. The results are seen in Figure 4.14. It is seen that for O-covered surfaces, the situation of the dopant occupying the surface CUS site is often more stable. This indicates that during OER, there is a driving force for moving dopants towards the surface CUS. Such driving forces also exist for several of the bare surfaces. The existence of such a driving force could be an explanation for the gradual removal of Ru from DSA electrodes during use[222, 223]. Experimental studies have shown that the degradation of DSAs is directly tied to the rate of OER[224–228], during which Electronic adsorption energy / eVPDF Image | Studies of Electrode Processes in Industrial Electrosynthesis
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