| Summary: | Due to the feasibility of an electrically rechargeable zinc/air cell made of a zinc foil as active material, an aqueous choline acetate (ChAcO) mixture as an electrolyte and a spinel MnCo<sub>2</sub>O<sub>4</sub> (MCO) and NiCo<sub>2</sub>O<sub>4</sub> (NCO) as a bi-functional oxygen catalyst was investigated in this work. The 30 wt.% water-containing aqueous ChAcO solution showed high contact angles close to those of KOH favoring triple-phase boundary formation in the gas diffusion electrode. Conductivity and pH value of 30 wt.% H<sub>2</sub>O/ChAcO amounted to 5.9 mS cm<sup>−1</sup> and 10.8, respectively. Best results in terms of reversible capacity and longevity of zinc/air cell were yielded during 100 h charge/discharge with the MnCo<sub>2</sub>O<sub>4</sub> (MCO) air electrode polarization procedure at 100 µA cm<sup>−2</sup> (2.8 mA g<sup>−1</sup><sub>zinc</sub>). The corresponding reversible capacity amounted to 25.4 mAh (28% depth of discharge (DOD)) and the energy efficiency ranged from 29–54% during the first and seventh cycle within a 1500 h polarization period. Maximum active material utilization of zinc foil at 100 µA cm<sup>−2</sup> was determined to 38.1 mAh (42% DOD) whereas a further charging step was not possible due to irreversible passivation of the zinc foil surface. A special side-by-side optical cell was used to identify reaction products of the zinc/air system during a single discharge step in aqueous ChAcO that were identified as Zn(OH)<sub>2</sub> and ZnO by Raman analysis while no carbonate was detected.
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