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ACTA MATERIALIA · 2025 · IF 9.3

In3Li13(311)/Li(110) coherent heterogeneous induced uniform epitaxial electrodeposition enabling the stable ultrathin lithium metal anode

An Wang,Shaozhen Huang,Zhangdi Xie,Jiahua Liao,Wenhao Li,Yuejiao Chen,Huimiao Li,Zhe Wang,Zhibin Wu,Libao Chen

A growing need for high-energy-density lithium metal batteries appeal for utilize ultrathin (≤50 μm) free-standing Li metal anodes . However, challenges such as the formation of an unstable solid electrolyte interphase and the lithium dendrites growth have led to poor cycling performance and safety concerns, limiting the commercial viability of thin lithium metal anodes. This work introduces a facile approach by designing and fabricating an ultrathin Li-In alloy anode through in-situ vacuum melting and codirectional continuous rolling. The rolled ultrathin Li-In anode achieves the induction of uniform epitaxial electrodeposition of Li(110), which is attributed to the lithiophility of the densely distributed In₃Li₁₃ alloy phase and the coherent heterogeneous relationship between textured In₃Li₁₃(311) and Li(110).The symmetrical cell assembled by 50 μm Li-In alloy anode exhibits a prolonged lifespan for 1800 h under the conditions of 1 mA cm -2 and 3 mAh cm -2 . Meanwhile, the LiFePO 4 ||Li-In (50 μm) full cell achieves sTable 450 cycles with a retention of 90.3 % at 2 C (1 C = 170 mA g -1 ). This work paves the path for the practical ultrathin Li anode for commercializing the lithium metal batteries .

CAS / MDL: 7440-74-6
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Energy Storage Materials · 2022 · IF 20.831

In-situ generated Li3N/Li-Al alloy in reduced graphene oxide framework optimizing ultra-thin lithium metal electrode for solid-state batteries

Jiaqi Zhu,Dan Cai,Jingru Li,Xiuli Wang,Xinhui Xia,Changdong Gu,Jiangping Tu

Optimization of lithium metal anode is a pivotal part in facilitating the evolution of next-generation high energy density solid-state lithium metal batteries (LMBs). However, the practical application of lithium anode in solid-state LMBs is limited by uncontrollable dendrite growth and the poor interfacial contact with solid electrolyte. Herein, a 40 µm thin lithium composite anode based on the AlN-embedded reduced graphene oxide (rGO) scaffold synthesized via one-step molten lithium infusion is proposed. The resulting lithiophilic Li-Al alloy and high ion-conductive Li 3 N in situ constructed the lithium ion diffusing highways inside electrode, enabling a well-oriented Li deposition and effectively inhibiting the dendrite growth. Combined with in-situ polymerization and Li 3 N-modified solid electrolyte interphase (SEI), the composite anodes can prolong the lifespan of symmetric cell to 2100 h at 0.2 mA cm −2 /0.2 mAh cm −2 in carbonate-based solid polymer electrolytes. Moreover, LAG||LiFePO 4 full cells also excelled in cycling capability and rate performance. This modified electrode offers a promising synergistic solution for designing high-performance solid-state LMBs.

研究领域: 材料科学 · 储能 · 电化学 · 固态电池 · 纳米材料
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Journal of Physical Chemistry Letters · 2023 · IF 5.7

All-Solid-State Batteries with Pre-plated Ultrathin Lithium Metal Enabled by No Pressure Holding and Characterized by In Situ Electron Paramagnetic Resonance Imaging

Ying Jiang,Guozhong Lu,Shinuo Kang,Fushan Geng,Bingwen Hu

All-solid-state batteries with ultrathin lithium metal, close to the anode-free solid-state batteries, could achieve high energy density. However, it is not trivial to plate an ultrathin lithium metal layer on a Cu current collector (Cu-CC). In situ electron paramagnetic resonance (EPR) imaging showed that the pre-plating on Cu-CC in a Li–In|Li6PS5Cl|Cu cell without pressure holding produced a lithium metal layer with a small area. However, when a Li–In|Li6PS5Cl|Cu cell was held under a considerable pressure, this cell would produce a lithium metal layer with a large area. The Cu-CC with the ultrathin lithium metal layer of a small surface could be extracted and then assembled with LiNiO2 and Li6PS5Cl to achieve better electrochemical performance compared to that of a large surface, because a small area of the lithium metal layer would lead to fewer side reactions and less consumption of lithium ions. This work suggests the importance of the control of the lithium plating and the observation of lithium plating by in situ EPR imaging.

研究领域: 材料科学 · 电化学 · 储能技术 · 固态电池技术
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ADVANCED MATERIALS · 2025 · IF 26.8

Engineering Stress-Potential Coupled Interface on Ultrathin Lithium Anodes Toward 450 Wh Kg−1-Level Long-Cycling Lithium Metal Batteries

Shaozhen Huang,Tianbao Li,Zhangdi Xie,Kun Li,Yuejiao Chen,Lin Mei,Gui-Chao Kuang,Zhibin Wu,Yu Zhang,Lin Gu,Libao Chen

Dendrite-free lithium anodes are crucial for developing practical high-energy-density batteries (>400 Wh/kg) with extended cycle life, but conventional interface design lack self-adaptive adjustment against dendrite growth during Li plating. Herein, we obtain a dendrite-free ultrathin Li@FcCHO anode by engineering a stress-responsive nano-interface on lithium strips via a mechanochemical reaction between ferrocene carboxaldehyde (FcCHO) and metallic Li. As proved by in situ Kelvin probe force microscopy and scanning electrochemical microscopy tests, the Li@FcCHO anode shows local potential response to the Li plating stress. Furthermore, density functional theory calculations show that the local surface potential change originates from stress-induced redistribution of anion-pair coordination. The stress-potential coupled interface layers induce uniform and dendrite-free Li deposition beneath the interface by suppressing dendritic Li from capturing Li + with the extra electric field. As a result, the Li@FcCHO anode exhibits ultralong cycling life over 5000 h under high areal capacity conditions, whilst a practical 452 Wh/kg pouch cell (9 Ah) based on the Li@FcCHO anode can survive over 470 cycles with capacity retention of 85.20%. This work pioneers a stress-potential coupled interface design to advance practical ultrathin Li anodes for next-generation high-energy-density batteries.

研究领域: 材料科学 · 储能 · 电化学 · 电池技术 · 纳米材料
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