This study addresses a fundamental challenge posed by hexavalent iron electrochemical irreversibility, which had slowed practical development of reversible Fe(VI) cathodes; nanolayers circumvent fundamental passivation challenges, and are electrodeposited from solution phase FeO42−, forming 601 mAh g−1 Li, and 485 mAh g−1 Na, Fe(III/VI) alkaline cathodes, the latter exhibiting 100–200 storage cycles at 80% depth of discharge, providing pathways towards metal hydride batteries with twice the cathode capacity.
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