Abstract
Unveiling the electrochemistry of solid-state Li2ZrCl6 halide electrolyte, we reveal its triple function as an ion conductor and a supplementary reversible, and sacrificial, electron source/sink. This groundbreaking discovery leads to a remarkable long-term enhancement of the specific capacity of industry-relevant heavily loaded LiFePO4 electrodes by several tens of percent, while significantly amplifying that of Si-based or anode-less full cells through effective compensation for side reactions. We show that these effects can potentially be tuned by adjusting the initial xLiCl-ZrCl4 composition of the solid electrolyte, which may thus become a new and mighty parameter for balancing the two electrodes.
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