Rechargeable Li-metal batteries using high-voltage cathodes can deliver the highest possible energy densities among all electrochemistries. However, the notorious reactivity of metallic lithium as well as the catalytic nature of high-voltage cathode materials largely prevents their practical application. Here, we report a non-flammable fluorinated electrolyte that supports the most aggressive and high-voltage cathodes in a Li-metal battery. Our battery shows high cycling stability, as evidenced by the efficiencies for Li-metal plating/stripping (99.2%) for a 5 V cathode LiCoPO (~99.81%) and a Ni-rich LiNiMnCoO cathode (~99.93%). At a loading of 2.0 mAh cm, our full cells retain ~93% of their original capacities after 1,000 cycles. Surface analyses and quantum chemistry calculations show that stabilization of these aggressive chemistries at extreme potentials is due to the formation of a several-nanometre-thick fluorinated interphase.
Li metal is regarded as the ''Holy Grail'' electrode because of its highest specific capacity and lowest electrochemical potential. However, challenges arising from the low Coulombic efficiency (CE) and dendritic nature of Li metal in carbonate electrolytes remain to be resolved. Here, by increasing LiFSI salt concentration in the carbonate electrolyte, we successfully increased the CE to 99.3% while suppressing Li dendrite formation. An NMC622jjLi cell was paired and showed excellent cycling performance.
Rechargeable alkaline zinc-air batteries promise high energy density and safety but suffer from the sluggish 4 electron (e−)/oxygen (O2) chemistry that requires participation of water and from the electrochemical irreversibility originating from parasitic reactions caused by caustic electrolytes and atmospheric carbon dioxide. Here, we report a zinc-O2/zinc peroxide (ZnO2) chemistry that proceeds through a 2e−/O2 process in nonalkaline aqueous electrolytes, which enables highly reversible redox reactions in zinc-air batteries. This ZnO2 chemistry was made possible by a water-poor and zinc ion (Zn2+)–rich inner Helmholtz layer on the air cathode caused by the hydrophobic trifluoromethanesulfonate anions. The nonalkaline zinc-air battery thus constructed not only tolerates stable operations in ambient air but also exhibits substantially better reversibility than its alkaline counterpart.
Efficient, rechargeable Mg and Ca batteries
Divalent rechargeable metal batteries such as those based on magnesium and calcium are of interest because of the abundance of these elements and their lower tendency to form dendrites, but practical demonstrations are lacking. Hou
et al
. used methoxyethyl amine chelants in which the ligands attach to the metal atom in more than one place, modulating the solvation structure of the metal ions to enable a facile charge-transfer reaction (see the Perspective by Zuo and Yin). In full battery cells, these components lead to high efficiency and energy density. Theoretical calculations were used to understand the solvation structures. —MSL
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