Abstract

Reducing SF6 (as gas cathode) in Li batteries is a promising concept for the double benefit of mildly converting greenhouse SF6 and providing a high theoretical energy density of 3922Wh kg-1 . However, the reduction process is hampered by its sluggish kinetics. Here, cobalt phthalocyanine (CoPc) molecules immobilized on porous carbon matrix are, for the first time, introduced to the LiSF6 chemistry to deliver an enhanced energy density. It is revealed that the high redox potential of Co(II)Pc/[Co(I)Pc]- (≈2.85V) facilitates the formation of Co(I)N4 sites to catalyze the SF6 electrochemical reduction. By using highly porous holey nitrogen-doped carbon nanocages as carbon matrix, the LiSF6 cells deliver a high discharge voltage of 2.82V at 50mA gC+CoPc -1 and an unprecedented areal capacity of 25 mAh cm-2 at 0.1mA cm-2 , much superior to previous results. This work opens up new possibilities for high-efficiency conversion of SF6 in lithium batteries.

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