1.吉林师范大学功能材料物理与化学教育部重点实验室,吉林 四平 136000
2.中国科学院深圳先进技术研究院,广东 深圳 518055
王旭昊(2002—),男,硕士研究生,研究方向为锂离子/锂金属负极材料,E-mail:15504348312@163.com;
郎集会,教授,研究方向为高熵合金、储能材料,E-mail:jhlang@jlnu.edu.cn
吴唯,助理研究员,研究方向为储能电极材料与高能量密度器件,E-mail:w.wu1@siat.ac.cn。
收稿:2025-10-23,
修回:2025-12-23,
纸质出版:2026-04-28
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本研究提出一种Li
2
S掺杂调控策略,通过熔融涂布制备10 μm超薄Li@Li
2
S复合锂箔,实现高能量密度、长循环锂金属电池的高效构建。Li
2
S与铜基底间较低的界面形成能显著改善熔融锂对铜的润湿性,助力超薄锂箔的大面积、高效率制备。同时,Li
2
S掺杂在改善锂负极对锂离子和电解液中锂盐阴离子的吸附能力、有效抑制枝晶生长并提升锂沉积均匀性的同时,协同诱导富无机组分固体电解质中间相膜的优先形成。该复合锂箔与高负载正极在负极/正极面容量比
<
1的少锂型锂金属电池体系中均展现出优异的循环稳定性,其中Li@Li
2
S||Ni92软包全电池(正极负载22.9 mg/cm
2
,面容量4.6 mAh/cm
2
)兼具超高能量密度(520 Wh/kg,1350 Wh/L)及长循环性能(0.2 C循环50次容量保持率99.8%)。这种“界面能-吸附能”双调控策略,既有效解决了纯锂熔融涂布过程中润湿性差、厚度不均等技术难题,还为电化学循环中的锂沉积行为和表面膜成分提供了良好的调控基础,有望为高比能、长循环锂金属电池的实用化突破提供低成本、可规模化的新路径。
This study proposes a Li
2
S doping strategy to fabricate 10 μm ultrathin Li@Li
2
S composite Li foils via molten casting
enabling the efficient construction of high-energy-density and long-cycle lithium meta
l batteries (LMBs). The low interfacial formation energy between Li
2
S and the Cu substrate improves the wettability of molten Li on Cu
allowing large-area
continuous preparation of ultrathin Li foils. Meanwhile
Li
2
S doping enhances the adsorption of Li ions and electrolyte anions on the Li anode
suppressing dendrite growth
improving Li deposition uniformity
and synergistically promoting the preferential formation of an inorganic-rich solid electrolyte interphase. The composite Li foil exhibits excellent cycling stability with high-loading cathodes in Li-limited LMBs with a negative/positive (N/P) areal capacity ratio
<
1. Notably
the Li@Li
2
S||Ni92 pouch full cell (cathode loading = 22.9 mg/cm
2
areal capacity = 4.6 mAh/cm
2
) achieves ultrahigh energy density (520 Wh/kg
1350 Wh/L) and long-cycle performance (99.8% capacity retention after 50 cycles at 0.2 C). This "interfacial energy-adsorption energy" dual-regulation strategy resolves poor wettability and uneven thickness in pure Li molten casting while favorably modulating Li deposition and surface film composition in subsequent electrochemical cycles
offering a low-cost
scalable pathway for practical high-energy-density
long-cycle LMBs.
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