Anode-free lithium–sulfur batteries (AFLSBs) show
a surprisingly
prolonged cycle life 2-fold higher than anode-free lithium metal batteries.
The principal difference is the presence of an intrinsic polysulfide
(PS) shuttle between electrodes in AFLSBs. However, the underlying
mechanism for the impact of PS redox species on the electrochemical
performance of AFLSBs is not clearly understood. Herein, we investigate
the role of PS redox species in retrieving inactive lithium for compensating
lithium inventory loss using titration gas chromatography, thereby
quantifying inactive lithium accumulated after several cycles. Moreover,
XPS analysis reveals reduced lithium sulfide (Li2S/Li2S2) species formed through PS redox shuttle refresh
inactive solid electrolyte interface (SEI) composition and stabilize
the consecutive cycle lithium deposition. Interestingly, synchrotron-based operando transmission X-ray microscopy (TXM) reveals dense
and granular electrodeposited lithium morphologies in AFLSBs. Therefore,
the interplay between reviving inactive lithium for compensating lithium
inventory loss and stabilizing lithium electrodeposition endows high
electrochemical performance in AFLSBs.
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