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Designing Solid Electrolyte Interfaces towards Homogeneous Na Deposition: Theoretical Guidelines for Electrolyte Additives and Superior High‐Rate Cycling Stability

A new 1,2-dibromobenzene (1,2-DBB) electrolyte additive is developed to accelerate Na ion diffusion through the solid electrolyte interphase layer and induce spherical Na deposition for dendrite-free Na metal anode due to the derived NaBr with high ionic conductivity. As enabled by the 1,2-DBB additive, the Na||Na3V2(PO4)3 full cells exhibit excellent long-term cycling performance.


Metallic Na is a promising metal anode for large-scale energy storage. Nevertheless, unstable solid electrolyte interphase (SEI) and uncontrollable Na dendrite growth lead to disastrous short circuit and poor cycle life. Through phase field and ab initio molecular dynamics simulation, we first predict that the sodium bromide (NaBr) with the lowest Na ion diffusion energy barrier among sodium halogen compounds (NaX, X=F, Cl, Br, I) is the ideal SEI composition to induce the spherical Na deposition for suppressing dendrite growth. Then, 1,2-dibromobenzene (1,2-DBB) additive is introduced into the common fluoroethylene carbonate-based carbonate electrolyte (the corresponding SEI has high mechanical stability) to construct a desirable NaBr-rich stable SEI layer. When the Na||Na3V2(PO4)3 cell utilizes the electrolyte with 1,2-DBB additive, an extraordinary capacity retention of 94 % is achieved after 2000 cycles at a high rate of 10 C. This study provides a design philosophy for dendrite-free Na metal anode and can be expanded to other metal anodes.

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