Ultra-High Discharge Voltage Plateau of 3.2 V Achieved in Li-CO2 Batteries Using Iron Polyphthalocyanine
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Rechargeable Li-CO 2 batteries offer great potential for greenhouse gas utilize and high-energy-density storage. However, their practical application is hindered by the formation of thermodynamically stable Li 2 CO 3 product that is hard to decompose during charging. Highly crystalline and conductive reticular material iron-polyphthalocyanine (pFe ‖ Pc) as solid-phase redox mediator into Li-CO 2 batteries tailors the cathode reaction pathway, enabling stable Li 2 C 2 O 4 generation and an extraordinary discharge plateau of 3.2 V beyond the theoretical limit. Beyond delivering an ultrahigh discharge capacity of 28790 mAh g -1 and reversible cyclability over 1400 hours (1000 mAh g -1 cut-off capacity) at 100 mA g -1 , the Li-CO 2 batteries exhibit excellent temperature adaptability (-40 to 80°C). The Li-CO 2 pouch cells employing pFe‖Pc as solid-phase redox mediator achieve a high energy density of 678 Wh kg -1 based on total device mass and maintain reversible cycling for 251 hours. Our work pioneers a promising pathway toward practical high-efficiency Li-CO 2 batteries.
