Excessive overpotential during charging is a major hurdle in lithium-oxygen (Li-O) battery technology. NO/NO redox mediation is an efficient way to substantially reduce the overpotential and to enhance oxygen efficiency and cycle life by suppressing parasitic reactions. Considering that nitrogen dioxide (NO) is a gas, it is quite surprising that NO/NO redox reactions can be sustained for a long cycle life in Li-O batteries with such an open structure. A detailed study with in situ differential electrochemical mass spectrometry (DEMS) elucidated that NO could follow three reaction pathways during charging: (1) oxidation of LiO to evolve oxygen, (2) vaporization, and (3) conversion into NO. Among the pathways, LiO oxidation occurs exclusively in the presence of LiO, which suggests that NO has high reactivity to LiO. At the end of the charging process, most of the volatile oxidized couple (NO) is stored by conversion to a stable third species (NO), which is then reused for producing the reduced couple (NO) in the next cycle. The dominant reaction of LiO oxidation involves the temporary storage of NO as a stable third species during charging, which is an innovative way for preserving the volatile redox couple, resulting in a sustainable redox mediation for a high-performance Li-O battery.
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