Molecular-Level Dual-Ionophilic Passivation for High-Areal-Capacity Lithium Metal Anodes on Nanostructured Paper Electrodes

IF 18.5 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Jisoo Kim, Yeong Hoon Heo, Jeonghun Lee, Son Ha, Jimin Park, Jong Chan Hyun, Minhyuck Park, Dong Hyuk Kang, Jung Hoon Kim, Hyoung-Joon Jin, Joong Tark Han, Young Soo Yun
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Abstract

Developing high-areal-capacity lithium metal anodes (LMAs) with exceptional reversibility, rapid charge-transfer kinetics, and long-term cycling stability remains a critical challenge for enabling next-generation high-energy-density lithium batteries. 2D electrodes suffer from poor rate performance and early lithium depletion at the electrode-electrolyte interface, while 3D architectures exhibit low Coulombic efficiency (CE) and excessive electrolyte consumption, compromising long-term stability. Herein, a nanostructured paper electrode (NPE) composed of oxygen-functionalized single-walled carbon nanotubes (Ox-SWCNTs) is introduced with a molecular-scale dual-ionophilic chitosan coating (C-NPE) to enhance LMA performance. The chitosan layer 1) reduces initial electrolyte decomposition to 1/25, 2) promotes an ultrathin, inorganic-rich solid-electrolyte-interface layer, and 3) increases active surface area and electrolyte uptake. At high areal capacity tests of 4.0 mA h cm⁻2, the high CE of >99.0% is achieved, and the overpotential is reduced by half, sustaining stable cycling for over 350 cycles—a tenfold increase compared to the premature failure observed in NPEs at 35 cycles. Furthermore, when integrated into Li–S batteries, C-NPE-based LMAs exhibit markedly suppressed polysulfide shuttling, mitigating capacity decay and overpotential-induced voltage drop. This enables a high energy density of 2385 Wh kg⁻¹ and a power density of 3475 W kg⁻¹, with stable operation over 150 cycles.

Abstract Image

纳米结构纸电极上高面积容量金属锂阳极的分子水平双亲离子钝化
开发具有优异可逆性、快速电荷转移动力学和长期循环稳定性的高面积容量锂金属阳极(lma)仍然是实现下一代高能量密度锂电池的关键挑战。2D电极的速率性能较差,并且在电极-电解质界面处存在早期锂耗尽的问题,而3D结构的库仑效率(CE)较低,电解质消耗过多,影响了长期稳定性。本文提出了一种由氧功能化单壁碳纳米管(Ox-SWCNTs)组成的纳米结构纸电极(NPE),并采用分子尺度双亲离子壳聚糖涂层(C-NPE)来提高LMA性能。壳聚糖层1)将初始电解质分解降低到1/25,2)促进超薄,富含无机的固体电解质界面层,3)增加活性表面积和电解质吸收。在4.0 mA h cm - 2的高面容量测试中,达到了99.0%的高CE,过电位降低了一半,维持了350多个循环的稳定循环——与npe在35个循环中观察到的过早失效相比,增加了10倍。此外,当集成到Li-S电池中时,基于c - npe的LMAs表现出明显抑制多硫化物穿梭,减轻容量衰减和过电位引起的电压下降。这样可以实现2385 Wh kg⁻¹的高能量密度和3475 W kg⁻¹的功率密度,可以稳定运行150次以上。
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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
期刊介绍: Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.
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