Activating reversible carbonate reactions in Nasicon solid electrolyte-based Na-air battery via in-situ formed catholyte.

Park, Heetaek; Kang, Minseok; Lee, Donghun; Park, Jaehyun; Kang, Seok Ju; Kang, Byoungwoo · Nat Commun · 2024

basic_science · Level V

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Abstract

Out of practicality, ambient air rather than oxygen is preferred as a fuel in electrochemical systems, but CO<sub>2</sub> and H<sub>2</sub>O present in air cause severe irreversible reactions, such as the formation of carbonates and hydroxides, which typically degrades performance. Herein, we report on a Na-air battery enabled by a reversible carbonate reaction (Na<sub>2</sub>CO<sub>3</sub>·xH<sub>2</sub>O, x = 0 or 1) in Nasicon solid electrolyte (Na<sub>3</sub>Zr<sub>2</sub>Si<sub>2</sub>PO<sub>12</sub>) that delivers a much higher discharge potential of 3.4 V than other metal-air batteries resulting in high energy density and achieves > 86 % energy efficiency at 0.1 mA cm<sup>-2</sup> over 100 cycles. This cell design takes advantage of moisture in ambient air to form an in-situ catholyte via the deliquescent property of NaOH. As a result, not only reversible electrochemical reaction of Na<sub>2</sub>CO<sub>3</sub>·xH<sub>2</sub>O is activated but also its kinetics is facilitated. Our results demonstrate the reversible use of free ambient air as a fuel, enabled by the reversible electrochemical reaction of carbonates with a solid electrolyte.