4.8 Article

Nanomicellar Electrolyte To Control Release Ions and Reconstruct Hydrogen Bonding Network for Ultrastable High-Energy-Density Zn-Mn Battery

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 145, Issue 36, Pages 20109-20120

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.3c07764

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A novel nanomicellar electrolyte using methylurea (Mu) has been developed to guide the homogeneous deposition of Zn2+ / Mn2+ and inhibit water-splitting-derived side reactions. The modified electrolyte also enhances the reversibility of the Mn2+ / MnO2 conversion reaction by regulating interfacial wettability and improving nucleation kinetics. These improvements result in extended cyclic stability, suppressed dendrites growth, exceptional capacity retention, and a high energy density in Zn-Mn batteries.
Zn-Mn batteries with two-electron conversion reactions simultaneously on the cathode and anode harvest a high voltage plateau and high energy density. However, the zinc anode faces dendrite growth and parasitic side reactions while the Mn2+/ MnO2 reaction on the cathode involves oxygen evolution and possesses poor reversibility. Herein, a novel nanomicellar electrolyte using methylurea (Mu) has been developed that can encapsulate ions in the nanodomain structure to guide the homogeneous deposition of Zn2+/Mn2+ in the form of controlled release under an external electric field. Consecutive hydrogen bonding network is broken and a favorable local hydrogen bonding system is established, thus inhibiting the water-splitting-derived side reactions. Concomitantly, the solid-electrolyte interface protective layer is in situ generated on the Zn anode, further circumventing the corrosion issue resulting from the penetration of water molecules. The reversibility of the Mn2+/MnO2 conversion reaction is also significantly enhanced by regulating interfacial wettability and improving nucleation kinetics. Accordingly, the modified electrolyte endows the symmetric Zn?Zn cell with extended cyclic stability of 800 h with suppressed dendrites growth at an areal capacity of 1 mAh cm(-2). The assembled Zn-Mn electrolytic battery also demonstrates an exceptional capacity retention of nearly 100% after 800 cycles and a superior energy density of 800 Wh kg(-1) at an areal capacity of 0.5 mAh cm(-2).

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