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In Situ Formation of Nitrogen‐Rich Solid Electrolyte Interphase and Simultaneous Regulating Solvation Structures for Advanced Zn Metal Batteries

A bifunctional electrolyte additive, N-Methyl pyrrolidone (NMP), is developed to improve the electrochemical performance of Zn anodes. NMP not only alters the solvation structure of Zn2+, but also in situ produces a dense nitrogen-rich layer on Zn. This layer protects Zn from corrosive electrolytes and benefits the uniform plating/stripping of Zn.


Abstract

Zn metal as one of promising anode materials for aqueous batteries suffers from notorious dendrite growth, serious Zn corrosion and hydrogen evolution. Here, a bifunctional electrolyte additive, N-methyl pyrrolidone (NMP), is developed to improve the electrochemical performance of Zn anode. NMP not only alters the solvation structure of Zn2+, but also in situ produces a dense N-rich solid-electrolyte-interphase layer on Zn foils. This layer protects Zn foils from corrosive electrolytes and benefits the uniform plating/stripping of Zn. Hence, the asymmetrical cells with NMP in the electrolyte retain a high coulombic efficiency of 99.8 % over 1000 cycles. The symmetric cells survive ≈200 h for 10 mAh cm−2 at a high Zn utilization of 85.6 %. The full cells of Zn||MnO2 show an impressive cumulative capacity even with lean electrolyte (E/C ratio=10 μL mAh−1), limited Zn supply (N/P ratio=2.3) and high areal capacity (5.0 mAh cm−2).

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