Storage and release of NO3− and I− via layered double hydroxide in carbonate electrolyte for stable lithium metal battery

Fenglin Wang; Zhicheng Zheng; Zuxin Wen; Wenqiang Fang; Chengwei Kuang; Fashen Chen; Hao Wan; Ning Zhang; Xiaohe Liu; Renzhi Ma; Gen Chen

doi:10.1016/j.scib.2025.04.016

論文 Storage and release of NO3− and I− via layered double hydroxide in carbonate electrolyte for stable lithium metal battery

Fenglin Wang ; Zhicheng Zheng ; Zuxin Wen ; Wenqiang Fang ; Chengwei Kuang ; Fashen Chen ; Hao Wan ; Ning Zhang ; Xiaohe Liu ; Renzhi Ma ; Gen Chen

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Fenglin Wang, Zhicheng Zheng, Zuxin Wen, Wenqiang Fang, Chengwei Kuang, Fashen Chen, Hao Wan, Ning Zhang, Xiaohe Liu, Renzhi Ma, Gen Chen. Storage and release of NO3− and I− via layered double hydroxide in carbonate electrolyte for stable lithium metal battery. Science Bulletin. 2025, 70 (15), 2493-2503. https://doi.org/10.1016/j.scib.2025.04.016

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(abstract)

The formation of inactive lithium (Li) in Li metal battery (LMB) primarily originates from the undesirable components of solid electrolyte interphase (SEI) and the growth of dendritic Li. LiNO3 has emerged as a promising electrolyte additive for mitigating interfacial instability and Li dendrite propagation through the in situ construction of nitride-rich SEI. However, the limited solubility of LiNO3 in carbonate electrolytes hinders its practical utilization. Herein, the bifunctional I−-MgAl layered double hydroxide (LDH) is proposed to synergistically dissolve LiNO3 and rejuvenate inactive Li. The anion-exchange capability of LDH facilitates the substitution of native I− with NO3−, forming NO3−-MgAl LDH and simultaneously generating I3−/I− redox mediators in electrolyte. This substitution not only achieves the dissolution of LiNO3, serving as a sustainable nitrogen source to optimize SEI components, but also enables the extracted I3−/I− redox couple to react spontaneously with inactive Li, remarkably enhancing the coulombic efficiency. Consequently, the engineered electrolyte significantly extends the lifespan of Li||LiFePO4, Li||NCM, and Li@Cu||LiFePO4 cells. The unique architecture of LDH can precisely control the storage and release of NO3− and I−, offering a transformative electrolyte design framework for next-generation batteries by integrating two-dimensional material properties with electrochemical mechanisms.

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