摘要:SummaryThe Ni-Fe battery is a promising alternative to lithium ion batteries due to its long life, high reliability, and eco-friendly characteristics. However, passivation and self-discharge of the iron anode are the two main issues. Here, we demonstrate that controlling the valence state of the iron and coupling with carbon can solve these problems. We develop a mesostructured carbon/Fe/FeO/Fe3O4hybrid by a one-step solid-state reaction. Experimental evidence reveals that the optimized system with three valence states of iron facilitates the redox kinetics, while the carbon layers can effectively enhance the charge transfer and suppress self-discharge. The hybrid anode exhibits high specific capacity of 604 mAh⋅g−1at 1 A⋅g−1and high cyclic stability. A Ni-Fe button battery is fabricated using the hybrid anode exhibits specific device energy of 127 Wh⋅kg−1at a power density of 0.58 kW⋅kg−1and maintains good capacity retention (90%) and coulombic efficiency (98.5%).Graphical abstractDisplay OmittedHighlights•A quaternary hybrid has been fabricated by a one-step solid-state reaction.•Controlling the valence state of iron facilitates redox kinetics and charge transfer.•The hybrid anode exhibits high specific capacity of 604 mAh⋅g−1at 1 A⋅g−1.•The NiFe battery exhibits specific energy of 127 Wh⋅kg−1and superior durability.Electrochemistry; Electrochemical energy storage; Engineering; Materials science; Energy materials