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Molecules 2021, 26, 2144 17 of 37 ratio and allowed better usage of strategic and expensive noble metals [12,156]. Even better results were observed for PdNi materials doped with phosphorus because of their enhanced activity and stability related to the presence of phosphorus [13,155] that, as a nonmetallic element, is capable of modifying the metals electronic structure, which enhances the electronic (ligand) effect related to the presence of nickel in PdNi catalyst [13]. Nickel itself can be used as a catalytic material. Because of its low price (compared to platinum), it has been proposed as the first nonprecious metal for alcohol oxidation and is gaining increasing research attention. The nickel surface characteristics, related to its oxidation from Ni2+ to Ni3+, lead to strong results in regard to the oxidation of simple alcohols [134]. During alcohol oxidation, Ni3+ is the active species, so the performance of nickel-based electrodes can be further improved using another element with low ox- idation potential as a dopant, which enhances the oxidation of nickel from the II to III oxidation state [134]. Examples of these elements include cobalt [134], chromium [129] and molybdenum [159]. In the case of a cobalt bifunctional mechanism takes place because Co atoms promote the adsorption of hydroxide ions at low potentials and thus improve the formation of nickel hydroxide active sites, as it was shown in reaction (10) [134]. Ni–Co–Fe has been used as an industrial-scale ethanol oxidation catalyst with the trade name HYPERMECTM [83,160]. The producer—an Italian company Enapter (previously called Acta) declares a peak performance of over 250 mW cm−2 at 80 ◦C with ethanol fuel and fuel cell durability over 3000 h for their noble metal-free catalyst [160]. They have also supplied electrodes for probably the world’s first fuel cell demonstration vehicle in cooperation with a team from the Hochschule Offenburg—the University of Applied Science in Germany at Shell Eco Marathon in France in 2006 [160]. The use of fuel cells as a power source for vehicles is very important because ethanol usage by the automotive industry is already increasing with the increasing participation of biodiesel, and further changes towards the elimination of fossil fuels would be much easier [83,160]. During its usage of HYPERMEC (Ni–Fe–Co catalyst), no acetate is found as a reaction product, and the formed acetaldehyde is further oxidized to carbon dioxide. Additionally, the lack of CO poisoning and higher current density obtained during the EOR with this system are large advantages compared to Pt-based catalysts [83]. The proposed reaction mechanism suggests that Ni sites are responsible for ethanol dehydrogenation and the breaking of the C–C bond, while Co and Fe are active sites for OH−-ion adsorption for further oxidation of ethanol decomposition fragments [83]. 3.3. Ethylene Glycol Oxidation Among the small organic molecules that can act as fuel for proton-exchange membrane fuel cells (PEMFCs), ethylene glycol is one of the most promising candidates. Ethylene glycol has low toxicity [28,90,161], low membrane penetration [25,85,90,108,161], high- energy-density [25,161] and relatively high reactivity in ambient temperatures [28,161], which are all valuable features for fuel in PEMFCs. It is a clear, odorless and biodegradable liquid that is very soluble in water [90]. Pure, anhydrous EG is not aggressive towards most metals and plastics, which, combined with low vapor pressure and stability, simplifies its transportation and storage. The only requirement for tank materials for ethylene glycol is that they cannot contain phenolic resins since they are not resistant to EG [90]. Additionally, EG is safer to work with than methanol and ethanol because it has a higher boiling point and higher volumetric capacity (see Table 1). Furthermore, because of the larger size of a single EG molecule, the membrane crossover is much smaller than in the case of methanol, which enhances the process efficiency because of the weaker cathodic poisoning effect [25,85,90,108]. The process of ethylene glycol production has been known since 1859, but its industrial- scale production began during World War I when it was used during the production of explosive materials as a substitute for glycerol [90]. Currently, it is a very important chemical that is widely used, i.e., in the automobile industry as a cooling agent [25,90,162] and as a raw material for the production of polyester fibers [90]. Nowadays, it is producedPDF Image | Effect of Anode Material on Electrochemical Oxidation of Alcohols
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