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

J Am Chem Soc

Key Laboratory of Precision and Intelligent Chemistry, and Department of Chemical Physics, University of Science and Technology of China, Jinzai Road 96, Hefei 230026, Anhui, China.

Published: September 2023


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Article Abstract

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 Mn/MnO 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 Zn/Mn 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 Mn/MnO 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. 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 at an areal capacity of 0.5 mAh cm.

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http://dx.doi.org/10.1021/jacs.3c07764DOI Listing

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