Defect-Modulated MOF Nanochannels for the Quasi-Solid-State Electrolyte of a Dendrite-Free Lithium Metal Battery

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Letters Pub Date : 2025-03-02 DOI:10.1021/acs.nanolett.4c05596

Jialong Jiang, Runhao Zhang, Jiachen Guo, Shiqi Zhang, Xiangtai Min, Ziyang Liu, Ning Liu, Dapeng Cao, Jun Xu, Peng Cheng, Wei Shi

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Abstract

Efficient and selective Li⁺ transport within the nanochannel is essential for high-performance solid-state electrolytes (SSEs) in lithium metal batteries. Introducing Li⁺ hopping sites into SSEs shows great potential for promoting Li⁺ transport; however, it typically reduces the Li⁺ transport nanochannel size, consequently increasing the energy barrier for Li⁺ transport. Herein, we present a molecular defect strategy for MOFs to introduce Li⁺ hopping sites and increase the nanochannel size simultaneously as quasi-solid-state electrolytes (QSSEs). Compared with the defect-free Li@UiO-66-based QSSE, the optimized Li@UiO-66-D2-based QSSE exhibits a remarkable 343% enhancement in Li⁺ conductivity and improved Li⁺ selectivity. Furthermore, the 9 cm × 6 cm Li|Li@UiO-66-D2|LFP pouch cell exhibits excellent cycling performance with high capacity retention. An in-depth mechanism study has unveiled the significant impact of both hopping sites and nanochannel size on Li⁺ transport, emphasizing the importance of a molecular defect strategy in enhancing the overall Li⁺ transport performance of MOF-based QSSEs.

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在锂金属电池的高性能固态电解质（SSE）中，纳米通道内高效和选择性的 Li+ 传输至关重要。在固态电解质中引入 Li+ 跳跃位点显示出促进 Li+ 输运的巨大潜力；然而，这通常会减小 Li+ 输运纳米通道的尺寸，从而增加 Li+ 输运的能量障碍。在此，我们提出了一种分子缺陷策略，即在 MOFs 中引入 Li+ 跳跃位点，同时增大纳米通道尺寸，使其成为准固态电解质（QSSEs）。与无缺陷的基于 Li@UiO-66 的 QSSE 相比，优化的基于 Li@UiO-66-D2 的 QSSE 的 Li+ 电导率显著提高了 343%，Li+ 选择性也得到了改善。此外，9 cm × 6 cm Li|Li@UiO-66-D2|LFP 袋式电池表现出优异的循环性能和高容量保持率。深入的机理研究揭示了跳跃位点和纳米通道尺寸对 Li+ 传输的重要影响，强调了分子缺陷策略在提高基于 MOF 的 QSSE 的整体 Li+ 传输性能方面的重要性。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.