Solvation Structure Engineering via Inorganic–Organic Composite Layer for Corrosion-Resistant Lithium Metal Anodes in High-Concentration Electrolyte

IF 24.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Advanced Energy Materials Pub Date : 2024-12-08 DOI:10.1002/aenm.202403944

Youngil Roh, Hyeokjin Kwon, Jaewon Baek, Changhoon Park, Seongyeong Kim, Kahee Hwang, A Reum Ha, Seongmin Ha, Jongchan Song, Hee-Tak Kim

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Abstract

High-concentration electrolytes have been reported to form an anion-derived, inorganic-rich solid electrolyte interphase on lithium metal electrodes; however, these electrodes suffer from high Li corrosion by the coordinated anions and consequent anion depletion. Herein, the study reports a composite layer comprising single-ion conducting ceramic (SICC) nanoparticles and a gel polymer electrolyte (GPE), which can suppress the Li corrosion in a high-concentration electrolyte based on lithium bis(fluorosulfonyl)imide (LiFSI) and a weakly solvating solvent (N,N-dimethylsulfamoyl fluoride, FSA). The lithium-ion space charges formed at the SICC/GPE interface reduce the coordination of anions in the composite layer, suppressing their decomposition. A Li | LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) pouch bi-cell with a composite layer-coated thin lithium metal anode (N/P = 1, thickness: 20 µm) delivers projected gravimetric (316 Wh kg⁻¹) and projected volumetric (1433 Wh L⁻¹) energy densities and exhibits stable operation for 350 cycles, with 70% capacity retention at 1/3 C charge–discharge rate. The engineering of the solvation structure through the inorganic–organic composite layer represents a practical strategy for developing corrosion-resistant lithium metal anodes in high-concentration electrolytes.

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高浓度电解液中耐腐蚀锂金属阳极的无机-有机复合层溶剂化结构工程

据报道，高浓度电解质在锂金属电极上形成阴离子衍生的富无机固体电解质界面；然而，这些电极受到配位阴离子的高锂腐蚀和随之而来的阴离子耗尽。本文报道了一种由单离子导电陶瓷（SICC）纳米颗粒和凝胶聚合物电解质（GPE）组成的复合层，该复合层可以抑制锂离子在高浓度双氟磺酰亚胺锂（LiFSI）和弱溶剂（N，N-二甲基磺酰氟，FSA）电解质中的腐蚀。在SICC/GPE界面形成的锂离子空间电荷降低了复合层中阴离子的配位，抑制了它们的分解。Li | LiNi0.8Co0.1Mn0.1O2 （NCM811）袋双电池具有复合层包覆的薄锂金属阳极（N/P = 1，厚度：20 μ m），可提供预计重量（316 Wh kg - 1）和预计体积（1433 Wh L - 1）能量密度，并在350次循环中稳定运行，在1/3 C充放电率下具有70%的容量保持率。通过无机-有机复合层实现溶剂化结构的工程化是在高浓度电解质中开发耐腐蚀锂金属阳极的一种实用策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Advanced Energy Materials CHEMISTRY, PHYSICAL-ENERGY & FUELS

CiteScore

41.90

自引率

4.00%

发文量

889

审稿时长

1.4 months

期刊介绍： Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small. With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics. The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.