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通过微小配位分散实现无枝晶锂金属负极的亲锂界面

Lithiophilic interface via tiny coordination dispersion enabling dendrite-free lithium metal anodes.

作者信息

Liu Chen, Zhang Wei, Yang Yiran, Xu Xinying, Li Ruhong, Ding Fei, Dai Changsong

机构信息

State Key Laboratory of Space Power-Sources, MOE Engineering Research Center for Electrochemical Energy Storage and Carbon Neutrality in Cold Regions, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China.

State Key Laboratory of Space Power-Sources, MOE Engineering Research Center for Electrochemical Energy Storage and Carbon Neutrality in Cold Regions, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China; YiChun Gotion Battery Co., Ltd, Yichun 336000, China.

出版信息

J Colloid Interface Sci. 2025 Nov 15;698:138050. doi: 10.1016/j.jcis.2025.138050. Epub 2025 Jun 1.

Abstract

Lithium metal batteries (LMBs) have emerged as promising candidates for next-generation high-energy-density systems. However, the practical implementation of LMBs faces critical challenges including uncontrolled dendrite proliferation and excessive lithium consumption, which significantly deteriorate cycling stability and raise safety concerns. To address these issues, a uniform and tiny S/P/Zn modified copper mesh (mCu@HCl-Zn-DDTP) is developed to regulate lithium plating behavior and prolong cycle lifespan. Acid-etching treatment provides enriched microinterfaces and additional sites for lithium deposition. Subsequently, coordination ensures adequate dispersion and transformation of S/P/Zn components via spatial segregation at the atomic scale. Benefiting from the synergistic effect of improved lithophilicity and enhanced inorganic components (LiS, LiP, LiO) in solid electrolyte interphase (SEI), the dendrite-free plating morphology is achieved and the irreversible reactions between lithium and electrolyte are effectively suppressed during cycling. Accordingly, the modified current collector enables exceptional cycling performance with 1000 stable cycles in half cells at 0.5 mA/cm. When paired with lithium iron phosphate (LFP) cathode, full cells demonstrate remarkable capacity retention exceeding 95 % after 500 cycles at 2C and 5C. This work provides a facile yet effective current collector engineering strategy that simultaneously addresses multiple interfacial challenges in LMBs, paving the way for practical high-energy-density battery applications.

摘要

锂金属电池(LMBs)已成为下一代高能量密度系统的有前途的候选者。然而,LMBs的实际应用面临着严峻挑战,包括枝晶无控制地生长和锂过度消耗,这显著降低了循环稳定性并引发安全问题。为了解决这些问题,开发了一种均匀且微小的硫/磷/锌修饰铜网(mCu@HCl-Zn-DDTP)来调节锂电镀行为并延长循环寿命。酸蚀处理提供了丰富的微界面和额外的锂沉积位点。随后,配位作用通过原子尺度的空间隔离确保了硫/磷/锌组分的充分分散和转化。受益于固体电解质界面(SEI)中改善的亲锂性和增强的无机成分(LiS、LiP、LiO)的协同效应,实现了无枝晶的电镀形态,并且在循环过程中有效抑制了锂与电解质之间的不可逆反应。因此,这种修饰的集流体在半电池中以0.5 mA/cm²的电流密度实现了1000次稳定循环的优异循环性能。当与磷酸铁锂(LFP)阴极配对时,全电池在2C和5C的电流密度下经过500次循环后显示出超过95%的显著容量保持率。这项工作提供了一种简便而有效的集流体工程策略,同时解决了LMBs中的多个界面挑战,为实际的高能量密度电池应用铺平了道路。

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