All‐Solid‐State Rechargeable Air Batteries with Naphthoquinone‐Based Negative Electrodes: Improved Performance and Cyclability

• Published in: Energy & environmental materials (Hoboken, N.J.) Vol. 8; no. 4
• Main Authors: Miyatake, Kenji, Wada, Suguru, Guo, Lin, Xian, Fang, Liu, Fanghua, Mahmoud, Ahmed Mohamed Ahmed, Yadav, Vikrant, Wong, Chun Yik
• Format: Journal Article
• Language: English
• Published: Hoboken Wiley Subscription Services, Inc 01.07.2025
• Subjects: Air batteries; all‐solid‐state batteries; Aqueous solutions; Batteries; Black carbon; Carbon; Carbon black; Charge efficiency; Conducting polymers; Discharge; Efficiency; Electrodes; Electrolytes; Ionomers; Membrane permeability; Membranes; naphthoquinone; Open circuit voltage; organic electrodes; Oxygen; Platinum; Polymers; Rechargeable batteries; Redox reactions; redox‐active compounds; Solid electrolytes; Voltage
• ISSN: 2575-0356; 2575-0356
• DOI: 10.1002/eem2.12887

All‐solid‐state rechargeable air batteries are designed and fabricated using 1,4‐naphthoquinone as a negative electrode, proton‐conductive polymer membrane as a solid electrolyte, and platinum‐based oxygen diffusion as a positive electrode as an emerging energy device. 1,4‐Naphthoquinone molecules exhibit reversible redox reactions peaked at 0.28 and 0.52 V versus reversible hydrogen electrode with the polymer electrolyte similar to that in an acid aqueous solution. The all‐solid‐state rechargeable air battery cell shows an open circuit voltage of 0.83 V, a nominal voltage of 0.3–0.4 V, a discharge capacity of 83.6 mAh g−1, and an initial Coulombic efficiency of 86.8%. The Coulombic efficiency after 15 charge–discharge cycles improves from 57.3% to 69.1% by replacing carbon black with graphite carbon as a support for the platinum catalyst in the positive electrode. Furthermore, replacing the commercial Nafion electrolyte membrane with the synthesized (in‐house) polyphenylene‐based ionomer (sulfonated polyphenylene‐quinquephenylene) electrolyte membrane improves the cycle durability of the resulting all‐solid‐state rechargeable air battery with high Coulombic efficiency retention (>98%) after 135 cycles owing to the lower oxygen permeability of the latter membrane. Overall, the present all‐solid‐state rechargeable air battery using 1,4‐naphthoquinone outperforms our previous all‐solid‐state rechargeable air battery using dihydroxybenzoquinene as a redox‐active molecule. This study reports all‐solid‐state‐rechargeable air batteries comprising redox‐active organic molecules (naphthoquinone) as negative electrodes, proton‐conductive polymer membranes as solid electrolytes, and platinum/carbon gas diffusion as positive electrodes. Naphthoquinone undergoes a reversible redox reaction in the solid state in the presence of small amount of water. Air batteries with the oxygen impermeable polymer membrane and corrosion‐resistive graphite carbon support for platinum catalysts show a discharge capacity of 81.7 mAh g−1, cyclability of >98%, CE of up to 135 cycles, and discharge rate properties of 4–100 C.