Yingyi Ding,Tianli Han,Zhao Wu,Yong Guan,Jun Hu,Chaoquan Hu,Yangchao Tian,Jinyun Liu
Magnesium/lithium hybrid-ion batteries (MLHBs) combine the advantages of high safety and fast ionic kinetics, which enable them to be promising emerging energy-storage systems. Here, a high-performance MLHB using a modified all-phenyl complex with a lithium bis(trifluoromethanesulfonyl)imide electrolyte and a NiCo2S4 cathode on a copper current collector is developed. A reversible conversion involving a copper collector with NiCo2S4 efficiently avoids the electrolyte dissociation and diffusion difficulties of Mg2+ ions, enabling low polarization and fast redox, which is verified by X-ray absorption near edge structure analysis. Such combination affords the best MLHB among all those ever reported, with a reversible capacity of 204.7 mAh g–1 after 2600 cycles at 2.0 A g–1, and delivers an ultrahigh full electrode-basis energy density of 708 Wh kg–1. The developed MLHB also achieves good rate performance and temperature tolerance at −10 and 50 °C with a low electrolyte consumption. The hybrid-ion battery system presented here could inspire a broad set of engineering potentials for high-safety battery technologies and beyond.
Stable cathodes with multiple redox-active centres affording a high energy density, fast redox kinetics and a long life are continuous pursuits for aqueous zinc-organic batteries. Here, we achieve a high-performance zinc-organic battery by tuning the electron delocalization within a designed fully conjugated two-dimensional hydrogen-bonded organic framework as a cathode material. Notably, the intermolecular hydrogen bonds endow this framework with a transverse two-dimensional extended stacking network and structural stability, whereas the multiple C = O and C = N electroactive centres cooperatively trigger multielectron redox chemistry with super delocalization, thereby sharply boosting the redox potential, intrinsic electronic conductivity and redox kinetics. Further mechanistic investigations reveal that the fully conjugated molecular configuration enables reversible Zn 2+ /H + synergistic storage accompanied by 10-electron transfer. Benefitting from the above synergistic effects, the elaborately tailored organic cathode delivers a reversible capacity of 498.6 mAh g −1 at 0.2 A g −1 , good cyclability and a high energy density (355 Wh kg −1 ).
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