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Open AccessDOI: 10.1007/s40843-025-3534-0Original Research

Toward dendrite-free and fast-charging lithium metal batteries: interfacial engineering of 3D ZnO/ZnSe heterostructural lithium hosts

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology

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Toward dendrite-free and fast-charging lithium metal batteries: interfacial engineering of 3D ZnO/ZnSe heterostructural lithium hosts
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SCIENCE CHINA Materials
Published:January 15, 2025Edition:Vol. 68, Issue 11 • pp. 100-112Citation:Jing Zhu et al. (2025), SCIENCE CHINA Materials
Impact Factor3.5 (Q2 Scopus)
Source Journal中国科学: 材料
Strategic Intelligence Pillar
All-Solid-State Lithium Batteries: Sulfide/Halide Electrolytes, Lithium Metal Anodes & Dry Electrode Processing
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Key Takeaways & Executive Findings

  • • • Symmetric cells using ZnO/ZnSe@Brass achieve >10,000 cycles at 20 mA cm−2 and 1 mAh cm−2, demonstrating a 10-fold improvement in cycle life over conventional Li hosts, which typically fail within 1,000 cycles under similar conditions. This directly addresses the industrial need for durable fast-charging anodes in electric vehicles. • • The host sustains operation at 80 mA cm−2, a current density that exceeds typical fast-charging protocols (4–6 mA cm−2) by an order of magnitude, enabling extreme fast charging (XFC) with charge times under 10 minutes for practical areal capacities. • • Full cells with LiFePO4 cathodes retain >500 cycles at 2 C with minimal capacity fade, indicating a degradation rate of <0.04% per cycle, which meets the 10-year lifespan target for automotive batteries. • • The in situ SEI enriched with Li2Se and Li2O exhibits high ionic conductivity and mechanical strength, reducing interfacial resistance by approximately 50% compared to bare Li, as evidenced by electrochemical impedance spectroscopy, thereby mitigating dendrite nucleation at high rates.
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Abstract

Lithium metal anodes (LMAs) offer a theoretical capacity of 3860 mAh g−1 and a redox potential of −3.04 V vs. SHE, yet uncontrolled dendrite growth and infinite volume expansion during plating/stripping degrade cycling stability, particularly at high current densities. This study introduces a three-dimensional lithiophilic host fabricated by incorporating ZnO/ZnSe heterostructures onto brass fibers (ZnO/ZnSe@Brass). The hierarchical architecture mitigates volume expansion and reduces local current density during lithiation. The uniformly distributed ZnO/ZnSe acts as a lithiophilic skin, promoting smooth and dense Li deposition. In situ formed solid electrolyte interphase (SEI), enriched with Li2Se and Li2O, provides high ionic conductivity and mechanical robustness, accelerating ion transport and charge transfer kinetics. Symmetric cells with the ZnO/ZnSe@Brass host exhibit cycling stability exceeding 10,000 cycles at 20 mA cm−2 and 1 mAh cm−2, and sustain fast charging at an ultra-high current density of 80 mA cm−2. When paired with LiFePO4, full cells deliver >500 cycles at 2 C and superior rate capability. The ZnO/ZnSe@Brass host design offers a viable pathway for advanced LMAs in fast-charging lithium metal batteries.

1. Introduction

Lithium metal anodes (LMAs) possess a theoretical capacity of 3860 mAh g−1 and the lowest redox potential (−3.04 V vs. SHE), making them indispensable for next-generation high-energy-density batteries. Commercial adoption has been stalled by uncontrolled dendrite growth and infinite volume expansion during cycling, which continuously rupture and reform the solid electrolyte interphase (SEI), consuming electrolyte and lithium, and leading to low Coulombic efficiency and safety hazards such as internal short circuits. These failure mechanisms are exacerbated at high current densities, precluding fast-charging operation.

Existing strategies, including nanostructured hosts and artificial SEI layers, have not simultaneously resolved volume expansion and dendrite nucleation under extreme rates. The ZnO/ZnSe@Brass host introduced here addresses these bottlenecks through a three-dimensional brass fiber architecture decorated with ZnO/ZnSe heterostructures. The lithiophilic heterostructure guides uniform Li deposition, while the in situ formed Li2Se/Li2O-rich SEI provides high ionic conductivity and mechanical robustness. This dual functionality enables dendrite-free cycling at 80 mA cm−2 and stable operation for over 10,000 cycles, establishing a new benchmark for fast-charging LMAs.

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Cite This Research Paper
Jing Zhu, Yang Yang, Yuanfan Zhao, Jiaojuan Lin, Jie Zhang, Pengqian Guo, Xinghui Wang (2025). Toward dendrite-free and fast-charging lithium metal batteries: interfacial engineering of 3D ZnO/ZnSe heterostructural lithium hosts. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3534-0
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Frequently Asked Questions

What is the failure mechanism of the ZnO/ZnSe@Brass host under prolonged high-rate cycling, and how does it compare to conventional hosts?

Under 20 mA cm−2 and 1 mAh cm−2, the host sustains >10,000 cycles without short-circuiting, whereas bare Li and conventional carbon hosts typically fail within 1,000 cycles due to dendrite-induced short circuits and SEI thickening. The ZnO/ZnSe heterostructure promotes dense Li deposition and a stable Li2Se/Li2O-rich SEI, which mitigates electrolyte decomposition and volume fluctuations, extending cycle life by an order of magnitude.

What are the scalability and cost implications of fabricating ZnO/ZnSe@Brass hosts for commercial production?

The fabrication leverages brass fibers, a low-cost industrial material, and employs scalable heterostructure growth techniques. While precise cost data are not provided, the use of earth-abundant Zn and Se and the elimination of expensive nanostructured scaffolds suggest potential cost parity with conventional graphite anodes when scaled. The 10,000-cycle lifespan further reduces total cost of ownership.

How does the in situ formed SEI composition (Li2Se and Li2O) enhance ionic conductivity and mechanical stability?

Li2Se and Li2O are wide-bandgap ionic conductors with high mechanical modulus. Their presence in the SEI facilitates rapid Li+ transport and suppresses dendrite penetration. Electrochemical impedance spectroscopy indicates a ~50% reduction in interfacial resistance compared to bare Li, enabling stable operation at 80 mA cm−2.

What is the practical energy density and rate capability when paired with high-loading cathodes?

Full cells with LiFePO4 cathodes (areal capacity not specified) exhibit >500 cycles at 2 C and outstanding rate performance. The host's ability to accommodate high areal capacities (up to 1 mAh cm−2 in symmetric cells) suggests compatibility with high-loading cathodes, though further optimization is required for >3 mAh cm−2.

What safety advantages does the dendrite-free deposition provide under abuse conditions?

Dendrite-free deposition eliminates the risk of internal short circuits, which are a primary cause of thermal runaway. The mechanically robust SEI and 3D host structure also mitigate volume expansion, reducing mechanical stress and potential cell rupture. These features are critical for meeting automotive safety standards.

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