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Molecules 2021, 26, 2144 23 of 37 Figure 7. Low- (A) and high-magnification (B) SEM images of dendrite-like PtAg nanocrystals, reprinted with permission of Elsevier [31]. The addition of two metallic, oxophilic elements lowers the water activation energy even more and thus lowers the EGOR onset potential [162]. For this reason, ternary systems, such as PtPdBi [88,154], PtRuNi, PtRuW and PtRuPd [162], have been developed. Such electrodes are more resistant to poisoning with carbon intermediates because of the optimal distribution of EG and OH species due to the presence of palladium and water activation on the bismuth atoms. When nickel is added to the PtSn system, this doping enhances the catalytic activity of the anode because of the changes in Pt electronic structure and NiO formation on the electrode surface, which results in a combination of the electronic effect and the bifunctional mechanism [162]. Compared to platinum catalysts, such electrodes lead to enhanced oxalate formation, which is linked to a lower surface tendency for catalyst poisoning with CO intermediates [88,154,162]. The second group of popular electrocatalytic materials for EGOR is based on palla- dium. Even though this metal is more abundant than platinum [22,36,39,183], its price is higher [22], but because of its unique catalytic properties and higher stability, this disad- vantage can be balanced by the higher efficiency of the oxidation processes [22]. During the oxidation of polyalcohols on the surface of palladium-based materials, higher peak current densities than in the case of platinum-based electrodes are observed, and the stability of such materials in alkaline media, which provide favorable conditions for such reactions, is remarkable [22,36,63,183]. Similar to other catalytic materials, the activity of palladium-based electrodes can be enhanced by doping with other elements that can either modify the surface process mecha- nism [63], such as the bifunctional mechanism [22,39] or change the electronic structure of the main metal [36,148,183,184], thus improving its catalytic performance. Other modifica- tions can be carried out by using highly conductive support materials, which can improve the electron transfer between the electrode and adsorbed molecules [36,183,185], or by preparing catalytic materials with high numbers of surface defects, which can improve the charge and mass transfer and decrease the energetic barriers in anodic materials [22,184]. Different doping metals change the reaction rate through different mechanisms. Dopants, such as bismuth [39,154] or nickel [22,186,187] in palladium result in a bifunc- tional mechanism that involves the oxidation of alcohol on the palladium atoms and water activation taking place on the surface of the doping elements. This provides the hydroxide ions necessary for complete alcohol oxidation. Different mechanisms of electrocatalytic activity enhancement are synergistic effects. These effects take place when doping ele- ments, such as iridium [188] or gold [36,57,189,190], induce an upshift in the palladium d-band center and thus result in stronger adsorption of hydroxide ions, which are crucial for complete alcohol oxidation [36,188,190]. This mechanism is similar to the electronic effect that takes place after doping with elements, such as copper [32,184], bismuth [39,154], iron [33,63,114,154,186] or ruthenium [24,39]. Instead of increasing the adsorption of hy- droxide ions, an electronic effect takes place; in the breaking of inter-carbon bonds, the charge transfer and desorption of CO-based intermediates are improved [24,39,184].PDF Image | Effect of Anode Material on Electrochemical Oxidation of Alcohols
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