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Li6PS5Cl
Journal of Physical Chemistry Letters · 2025 · IF 4.6

A Ring-Shaped Lithium Metal Anode Enables High-Performance All-Solid-State Batteries Revealed by In Situ L-Band EPR Imaging

Jiaxing Lv,Ying Jiang,Guozhong Lu,Xiaobing Lou,Bingwen Hu

In traditional operations of all-solid-state lithium metal batteries (ASSLMBs), a small thin lithium metal circular disk is employed as a lithium metal anode (LMA). However, ASSLMBs with a circular-disk LMA often fail in <150 cycles with low capacity retention. In this work, we developed a new ring-shaped LMA to improve cyclability. Full cells consisting of a ring-shaped LMA, a LiCoO2 cathode, and a Li6PS5Cl electrolyte maintain good capacity retention of 83.65% at 0.3C after 300 cycles. Moreover, in situ L-band electron paramagnetic resonance imaging (EPRI) showed that fewer Li dendrites are formed on a ring-shaped LMA. This work highlights the importance of the design of the shape of the LMA to mitigate the growth of lithium dendrites and shows that L-band EPRI is a useful technique for ASSLMBs.

CAS / MDL: 554-13-2
研究领域: 材料科学 · 电化学 · 储能技术 · 电池技术
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ACS Nano · 2023 · IF 17.1

Robust All-Solid-State Lithium Metal Batteries Enabled by a Composite Lithium Anode with Improved Bulk Li Diffusion Kinetics Properties

Shuxian Zhang,Jianchao Chen,Chunyan Zhu,Qingyuan Liu,Qingyu Li,Renbo Liu,Xiaobo Jiang,Yijie Yan,Shengjian Sun,Longwei Yin,Rutao Wang

All-solid-state batteries (ASSBs) with a Li metal anode are expected to be one of the most promising energy storage systems to achieve high energy density. However, the interfacial instability between the Li metal anode and solid-state electrolyte (SSE) limits the rate capability and cycling stability of ASSBs. The main issue is the formation of voids at the Li/SSE interface during Li stripping due to the slow diffusion of Li within the bulk Li metal, then increasing internal cell resistance and inducing the formation of lithium dendrites. To address these issues, a composite Li anode (LAO) composed by Li–Ag alloy and Li2O is constructed by mixing the stoichiometric metal Li and Ag2O directly. LAO anode is capable of improving bulk Li diffusion kinetics and inhibiting the formation of interfacial voids effectively, achieving a high critical current density over 1.5 mA cm–2 and long stable cycling over 1000 h at 1 mA cm–2. The ASSBs, employing LAO as the anode, Li6PS5Cl as the SSE, and LiCoO2 as the cathode, exhibit superior rate capability and stable cycling over 4000 cycles at 5 C. Moreover, ASSBs can operate stably with a high LiCoO2 loading of 17.8 mg cm–2 for more than 100 cycles at 0.2 C.

研究领域: 材料科学 · 电化学 · 能源存储
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Synergistic Defect Engineering and Interface Stability of Activated Carbon Nanotubes Enabling Ultralong Lifespan All-Solid-State Lithium–Sulfur Batteries

Cheng Wang,Yue Wu,Jing Gao,Xiaolin Sun,Qing Zhao,Wenyan Si,Yuan Zhang,Kun Wang,Fuhua Zhao,Takeo Ohsaka,Futoshi Matsumoto,Changshui Huang,Jianfei Wu

Due to the high energy density, high safety, and low cost of sulfur, all-solid-state lithium–sulfur batteries (ASSLSBs) are considered one of the most promising next-generation energy storage devices. Nevertheless, the insufficient interfacial contact between solid electrolytes (SEs) and the active material of sulfur leads to inadequate electronic and ionic conduction, which increases interfacial resistance and capacity decay. In this paper, commercial carbon nanotubes (CNTs) are activated to form porous-CNTs (P-CNTs), which are used as sulfur-bearing matrix, forming S@P-CNTs-based composite cathodes for ASSLSBs. Compared with CNTs, P-CNTs possess a larger specific surface area and more oxygen-containing groups, providing enhanced interfacial contact and stability between S@P-CNTs and Li6PS5Cl SE, which are confirmed by scanning electron microscopy, X-ray photoelectron spectroscopy, and density functional theory calculations. Moreover, P-CNTs can form a 3D conductive network in the composite cathodes, facilitating the migration of electrons and the diffusion of ions, as well as improving the utilization of sulfur. As a result, the S@P-CNTs-based ASSLSBs display excellent electrochemical performances, especially rarely reported ultralong lifespan, which deliver a capacity of 1099.2 mA h g–1 at a current density of 1.34 mA cm–2, and remarkably maintain 70.4% of the initial capacity over 1400 cycles.

研究领域: 材料科学 · 储能技术 · 纳米技术 · 电池技术
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CHINESE CHEMICAL LETTERS · 2023 · IF 9.1

Halide/sulfide composite solid-state electrolyte for Li-anode based all-solid-state batteries

Haochang Zhang,Zhaozhe Yu,Jinyin Cheng,Hannan Chen,Xiao Huang,Bingbing Tian

Li 2 ZrCl 6 (LZC) solid-state electrolytes (SSEs) have been recognized as a candidate halide SSEs for all-solid-state Li batteries (ASSLBs) with high energy density and safety due to its great compatibility with 4 V-class cathodes and low bill-of-material (BOM) cost. However, despite the benefits, the poor chemical/electrochemical stability of LZC against Li metal causes the deterioration of Li/LZC interface, which has a detrimental inhibition on Li + transport in ASSLBs. Herein, we report a composite SSE combining by LZC and argyrodite buffer layer (Li 6 PS 5 Cl, LPSC) that prevent the unfavorable interaction between LZC and Li metal. The Li/LPSC-LZC-LPSC/Li symmetric cell stably cycles for over 1000 h at 0.3 mA/cm 2 (0.15 mAh/cm 2 ) and has a high critical current density (CCD) value of 2.1 mA/cm 2 at 25 °C. Under high temperature (60 °C) which promotes the reaction between Li and LZC, symmetric cell fabricated with composite SSE also display stable cycling performance over 1200 h at 0.3 mAh/cm 2 . Especially, the Li/NCM ASSLBs fabricated with composite SSE exhibit a high initial coulombic efficiency, as well as superior cycling and rate performance. This simple and efficient strategy will be instrumental in the development of halide-based high-performance ASSLBs.

研究领域: 材料科学 · 电化学 · 能源存储
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Advanced Science · 2023 ·Vol. 10 ·期 32 ·2304117 · IF 15.1

One Stone, Three Birds: An Air and Interface Stable Argyrodite Solid Electrolyte with Multifunctional Nanoshells

Junwu Sang,Kecheng Pan,Bin Tang,Zhang Zhang,Yiyang Liu,Zhen Zhou

Li 6 PS 5 Cl (LPSC) solid electrolytes, based on Argyrodite, have shown potential for developing high energy density and safe all-solid-state lithium metal batteries. However, challenges such as interfacial reactions, uneven Li deposition, and air instability remain unresolved. To address these issues, a simple and effective approach is proposed to design and prepare a solid electrolyte with unique structural features: Li 6 PS 4 Cl 0.75 -OF 0.25 (LPSC-OF 0.25 ) with protective LiF@Li 2 O nanoshells and F and O-rich internal units. The LPSC-OF 0.25 electrolyte exhibits high ionic conductivity and the capability of “killing three birds with one stone” by improving the moist air tolerance, as well as the interface compatibility between the anode or cathode and the solid electrolyte. The improved performance is attributed to the peculiar morphology and the self-generating and self-healing interface coupling capability. When coupled with bare LiCoO 2 , the LPSC-OF 0.25 electrolyte enables stable operation under high cutoff voltage (≈4.65 V vs Li/Li + ), thick cathodes (25 mg cm −2 ), and large current density (800 cycles at 2 mA cm −2 ). This rationally designed solid electrolyte offers promising prospects for solid-state batteries with high energy and power density for future long-range electric vehicles and aircrafts.

研究领域: 材料科学 · 电化学 · 电池技术 · 储能技术
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