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Li2S
Journal of Materials Chemistry A · 2018 ·Vol. 6 ·期 21 ·9906-9914 · IF 9.931

A green and facile strategy for the low-temperature and rapid synthesis of Li2S@PC–CNT cathodes with high Li2S content for advanced Li–S batteries

Sheng Liang,Yang Xia,Chu Liang,Yongping Gan,Hui Huang,Jun Zhang,Xinyong Tao,Wei Sun,Weiqiang Han,Wenkui Zhang

Lithium sulfide (Li2S) is considered as a promising lithium storage material because of its high theoretical specific capacity of 1166 mA h g−1. The electrochemical performance of Li2S can be remarkably improved by introducing carbon to form Li2S–carbon composites. However, the complex preparation process of Li2S–carbon composites limits their large-scale applications. Herein, we present a green and facile strategy to synthesize porous carbon-coated Li2S–carbon nanotube composites (Li2S@PC–CNT) by heating carbon disulfide (CS2) and the lithium hydride–CNT mixture at a temperature below 250 °C, which is the lowest temperature for in situ synthesis of Li2S–carbon composites reported till date. For the Li2S@PC–CNT composites, Li2S@PC particles are connected with neighboring particles through the 3D CNTs network skeleton. This unique nanoarchitecture not only prevents the loss of active materials and diffusion of polysulfides, but also significantly facilitates fast electron and ion transport. As a result, a high specific capacity (820 mA h g−1 at 0.1 A g−1 after 10 cycles) and a remarkable cycle life (502 mA h g−1 at 0.5 A g−1 after 300 cycles) are achieved. The rationally designed structure and superior electrochemical performance of the Li2S@PC–CNT composites will pave a new avenue for realizing high energy density of Li–S batteries.

研究领域: 材料科学 · 电化学 · 纳米科技 · 能源存储 · 无机化学
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Journal of Energy Storage · 2024 · IF 8.9

Low-cost preparation and purification of Li2S for sulfide solid electrolytes

Yadong Wei,Zixiang Zhao,Liang Qi,Yue Ma,Hongzhou Zhang,Zhenyu Wang,Lianqi Zhang,Yongan Yang,Dawei Song

Lithium sulfide (Li 2 S) is a key raw material for synthesizing sulfide solid electrolytes (SSEs), which has been considered as one of the most promising solid electrolytes for all-solid-state lithium batteries (ASSLBs). However, the high cost of Li 2 S limits the development of SSEs. Herein, a novel approach for the preparation of Li 2 S through carbothermal reduction of lithium sulfate (Li 2 SO 4 ) is designed and optimized. Two novel strategies for purifying rough Li 2 S materials are proposed in this work. A low raw material cost of $148 kg −1 and a high yield of 88.50 % are achieved. Subsequently, Li 6 PS 5 Cl and Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 solid electrolytes are synthesized with the self-made Li 2 S and the corresponding electrochemical performances are evaluated. In NCMA|Li 6 PS 5 Cl|Li/In system, a high discharge capacity of 135 mAh g −1 is maintained after 500 cycles at 1C. In NCMA|Li 9.54 Si 1.74 P 1.44 S 11.7 Cl 0.3 |Li/In system, a high discharge capacity of 132 mAh g −1 is maintained after 350 cycles at 1C. The high capacity and long cycle life demonstrate the effectiveness of Li 2 S preparation and purification strategy proposed in this work.

研究领域: 材料科学 · 电化学 · 储能技术 · 固态电池 · 无机合成
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Small Methods · 2025 · IF 9.1

Li2S Cathode Mediated by Diphenyl Chalcogenides in All-Solid-State Batteries

Chenxin Huang,Junsheng Fan,Wenxuan Sun,Yongzhu Fu,Wei Guo

Lithium sulfide (Li 2 S), as one of the critical cathodes in all-solid-state batteries, shows promising potential. However, its ion and electron blocking characteristics necessitate a high charge overpotential for activation, which can result in the decomposition of sulfide-based solid-state electrolytes. In this study, diphenyl chalcogenides are applied as redox mediators to reduce the initial charge voltage and improve the utilization of Li 2 S in all solid-state lithium-sulfur batteries. Among them, diphenyl ditelluride (DPDTe) enables the highest initial charge capacity (963.1 mAh g −1 ) of Li 2 S. The Li 2 S-DPDTe composite cathode, along with Li 7 P 3 S 11 sulfide electrolyte and In-Li anode, exhibits a low charge voltage of 2.4 V. After 360 cycles, the battery demonstrates an average areal discharge capacity of 0.9 mAh cm −2 at a current density of 0.2 mA cm −2 (706.8 mAh g −1 based on the mass of Li 2 S). This study aims to use diphenyl chalcogenides as mediators to lower the initial overpotential of Li 2 S, thereby aligning with the narrow electrochemical window of sulfide electrolytes and providing valuable insights for high-energy-density all-solid-state batteries.

CAS / MDL: 103-29-7
研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 电池技术 · 功能材料
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ACS Applied Energy Materials · 2025 · IF 5.5

A Scalable Cathode Prelithiation Technique for Compensating the Initial Capacity Loss of Lithium-Ion Batteries

Hongqiang Zhang,Tiansheng Bai,Jun Cheng,Fengjun Ji,Yuxiang Qiu,Zhen Zeng,Yuanyuan Li,Chenwu Zhang,Jingyu Lu,Lijie Ci,Deping Li

Irreversible capacity loss during the initial charge–discharge process poses a significant challenge to the practical application of high-theoretical-capacity anodes in lithium-ion batteries. Therefore, prelithiation technology has emerged as a pivotal choice for the advancement of high-energy-density lithium-ion batteries. Herein, we introduce a bilayer coating strategy with Li2S-polyacrylonitrile (Li2S-PAN) as the prelithiation source. Specifically, Li2S-PAN can selectively release active lithium ions during the initial charge process with a specific capacity of 695 mAh g–1. When integrated into a LiFePO4 cathode, Li2S-PAN can achieve a 48.2% additional capacity. Furthermore, the LiFePO4|SiC full cell exhibits a ∼20.0% initial lithium compensation with the reversible capacity increasing from 101 to 121 mAh g–1. Overall, this work proposes a facile and scalable route for the future application of high-theoretical-capacity anodes (silicon, tin, etc.) in the lithium-ion battery industry.

CAS / MDL: 110-71-4
研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

“First-Cycle Effect” of Trace Li2S in a High-Performance Sulfur Cathode

Kai Yuan,Lixia Yuan,Jingwei Xiang,Yaqi Liao,Jie Chen,Yunhui Huang

Lithium–sulfur battery is one of the most promising choices for next-generation batteries due to its high theoretical energy density and natural abundance. However, the sulfur cathode undergoes a stepwise reduction process and generates multiple soluble polysulfide intermediates; for the further conversion from the dissolved intermediates to the final solid product (Li2S), the surface nucleation barrier limits the speed of the electrochemical precipitation, resulting in serious polysulfide diffusion loss and low sulfur utilization. Herein, the trace Li2S (tLi2S) is modified on the carbon fiber (CF) skeleton as preloaded crystal nuclei to boost the electrokinetics of Li2S deposition in the initial cycle. The trace Li2S decreases the nucleation barrier on the modified electrode (tLi2S@CF), resulting in a high initial capacity of 1423 mAh g–1 for the Li2S6 catholyte (0.2 C), which corresponds to a nearly 100% utilization of Li2S6. Furthermore, the trace Li2S nuclei induce a uniform distribution of the redeposited active materials, and the uniform distribution persists in the following cycles, which benefits the cycle life significantly. The sulfur cathode based on the tLi2S@CF matrix maintains a capacity of 1106 mAh g–1 at 1 C rate after 100 cycles. The strategy can provide a new avenue for the rational design of the sulfur cathode.

研究领域: 材料科学 · 电化学
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IONICS · 2019 ·Vol. 26 ·期 5 ·2335-2342 · IF 2.289

In situ generated Li2S-LPS composite for all-solid-state lithium-sulfur battery

Jiang Huize,Han Yu,Wang Hui,Guo Qingpeng,Zhu Yuhao,Xie Wei,Zheng Chunman,Xie Kai

Li 3 PS 4 (LPS) was in situ formed at the active material Li 2 S through the reaction of Li 2 S and P 2 S 5 by mechanical ball milling, which can be used to composite cathode for Li/S battery. The fine active materials-electrolyte interface will be generated via in situ reaction. Compared with the direct mixing Li 2 S + LPS, the interface impedance between Li 2 S and LPS of Li 2 S-LPS had a significant decrease from 833.3 Ω to 203.7 Ω at room temperature. The effect of heat treatment temperature on the ionic conductivities of Li 2 S-LPS has been studied, and the Li 2 S-LPS-300 showed the highest ionic conductivity of 2.67 × 10 −4 S cm −1 at room temperature. The all-solid-state cell (Li/LPS/Li 2 S-LPS) possessed a larger capacity and better rate performance than that of the cell using Li 2 S + LPS as cathode material, showing a discharge capacity of 624.5 mAh g −1 (g of Li 2 S) for the 20th cycle. We also find that high carbon content of composite cathode will reduce the utilization of Li 2 S. The composite cathode 90Li 2 S-LPS + 10C (wt%) shows the highest capacity of 763.8 mAh g −1 at the current density of 0.1 mA cm −2 .

研究领域: 材料科学 · 电化学 · 储能
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Low-Cost and Scalable Synthesis of High-Purity Li2S for Sulfide Solid Electrolyte

Fangyuan Tu,Zixiang Zhao,Xin Zhang,Zhenyu Wang,Yue Ma,Hongzhou Zhang,Dawei Song,Lianqi Zhang,Yongan Yang,Lingyun Zhu

Sulfide solid electrolytes (SSEs) are preferable for all-solid-state lithium batteries (ASSLBs) to achieve high energy densities. However, the development of SSEs is impeded due to the high cost of the key raw material─Li2S. It is of great significance to synthesize high-purity Li2S with a more accessible and economic method. Herein, a new strategy for large-scale synthesis of Li2S with a low cost is developed on the basis of a lithium sulfate carbothermic reduction reaction in this work. A high yield of 81.78% and low raw material cost of $62 kg1– are achieved, significantly lower than that of its commercial counterpart ($10,000–15,000 kg1–). To verify the effectiveness of this method, the as-prepared Li2S is further used to synthesize Li6PS5Cl (LPSC), and the corresponding electrochemical performances are evaluated. Room temperature ionic conductivity of LPSC reaches 2.63 mS cm–1. In the NCM622@Al2O3(NCM622@AlO)//LPSC//Li–In ASSLB system, a high discharge specific capacity of 136 mAh g–1 is maintained after 700 cycles at 1C with an ultrahigh area loading of 35.6 mg cm–2 (calculated according to NCM622@Al2O3, which is almost twice the other works). These performances are comparable to those using LPSC from expensive commercial Li2S in the control group, demonstrating the feasibility of the Li2S preparation strategy proposed in this work.

研究领域: 材料科学 · 储能 · 固态化学 · 电化学 · 电池技术
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CHEMICAL ENGINEERING JOURNAL · 2018 · IF 6.735

Constructing fast electron and ion conductive framework for Li2S as advanced lithium sulfur battery

Yueying Peng,Yiyong Zhang,Zhipeng Wen,Yunhui Wang,Zhiqiang Chen,Bing-Joe Hwang,Jinbao Zhao

Lithium sulfide (Li 2 S) cathode is considered as a prospective substitution for sulfur-based cathode for as its high specific capacity. Despite this, the poor electron and lithium ion transportation for Li 2 S impedes its further development. Herein, a great electron and lithium ion pathway is constructed for Li 2 S by a facile spray-dried technology. In this composite, the nano-sized Li 2 S is well imbedded in framework composed by the nitrogen/oxygen dual doped carbon nanotube/carbon (Li 2 S/CNT/C-N/O). The electrochemical tests show that the prepared Li 2 S/CNT/C-N/O cathode exhibits great cycling stability and rate capacity. A high initial discharge capacity of 1014 mAh g −1 is achieved with 671 mAh g −1 capacity remained at 200 mA g −1 after 200 cycles. Impressively, a stable capability is still exhibited from 200 to 3000 mA g −1 during rate testing. In-situ electrochemical impedance spectra test is further used to get insightful understanding about the improvements. The result reveals that decreased resistance and increased lithium-ion diffusion can be achieved for the Li 2 S/CNT/C-N/O, especially at the initial charging stage of polysulfides nucleation, which shed light on the improved reactive kinetics and active material utilization.

研究领域: 材料科学 · 电化学
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2019 ·Vol. 23 ·期 11 ·3145-3151 · IF 2.531

Li metal-free rechargeable all-solid-state Li2S/Si battery based on Li7P3S11 electrolyte

Xu Xiaoyan,Cheng Jun,Li Yuanyuan,Nie Xiangkun,Dai Linna,Ci Lijie

As high energy density and enhanced safety are required for the lithium-ion battery development, all-solid-state battery has attracted significant attention. Herein, we report an all-solid-state full battery consisting of a Li 7 P 3 S 11 solid electrolyte coated silicon anode, Li 2 S/graphene composite cathode, and Li 7 P 3 S 11 solid-state electrolyte. With a high capacity for the silicon anode and Li 2 S cathode, this battery yields a high theoretical specific energy density up to 1495 Wh kg −1 , which is higher than that of lithium-ion batteries based on oxide cathodes. Moreover, Li 2 S cathode is used as lithium source instead of using metallic lithium, avoiding interface reaction between lithium metal anode and sulfide electrolyte Li 7 P 3 S 11 . This all-solid-state battery system we proposed could avoid the safety issues associated with the use of lithium metal and be a promising candidate for an enhanced energy density, which would promote their applications in the fields of electric vehicles and portable electronics.

研究领域: 材料科学 · 储能 · 电化学 · 电池技术
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JOURNAL OF POWER SOURCES · 2015 · IF 6.217

Facile synthesis of porous Li2S@C composites as cathode materials for lithium–sulfur batteries

Sheng Liang,Chu Liang,Yang Xia,Haohui Xu,Hui Huang,Xinyong Tao,Yongping Gan,Wenkui Zhang

Lithium sulfide (Li 2 S) is regarded as a promising cathode material for lithium–sulfur (Li–S) batteries in terms of its high theoretical specific capacity of 1166 mAh g −1 and good compatibility with lithium metal-free anodes. However, Li 2 S suffers from poor cycling stability and rate capability resulted from the serious shuttle effect of lithium polysulfides and its low electronic and ionic conductivity . Here, we present a facile ball milling combined with carbon coating method to synthesize porous carbon-coated Li 2 S (Li 2 S@C) composites with a high Li 2 S content by using polystyrene (PS) as a carbon precursor. The Li 2 S@C composites show a high reversible specific capacity of 676 mAh g −1 (equal to 971 mAh g −1 sulfur) after 3 cycles at the current density of 0.1 A g −1 , superior cycling stability with an average decay rate of 0.18% per cycle over 200 cycles, and improved rate capability of 416 mAh g −1 at the current density of 1.0 A g −1 . The enhanced electrochemical properties of Li 2 S can be attributed to the porosity and core–shell structure of the Li 2 S@C composites, which increased the electronic and ionic conductivity of Li 2 S and alleviated the shuttle effect of intermediate lithium polysulfides in the discharge/charge process.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 功能材料
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2023 ·Vol. 28 ·期 7 ·2413-2423 · IF 2.5

Li2S@C/CNT composite cathode with botryoidal conductive network for advanced lithium–sulfur batteries

Lu Chengwei,Yu Liyue,Zhou Xiaozheng,Gan Yongping,He Xinping,Huang Hui,Zhang Jun,Zhang Wenkui,Xia Xinhui,Xiao Zhen,Fang Ruyi,Xia Yang

Lithium sulfide (Li 2 S) is a promising alternative cathodic material for lithium–sulfur batteries, which can alleviate the volume expansion of sulfur‑based cathodes. As a fully lithiated cathode, Li 2 S can be paired with Li-free anodes, thereby increasing the selectivity of anodic materials. Nevertheless, Li 2 S cathode is hindered by its high cost, harsh preparation conditions, and inadequate conductivity, which impose limitations on its practical application. Hence, the crucial factor in enabling the practicality of Li 2 S cathode is the development of low-cost and facile synthetic methods to produce highly conductive Li 2 S material. Herein, a high‑conductivity Li 2 S@C/CNT composite cathode is prepared using low-cost Li 2 SO 4 as a lithium source through a facile spray drying technique combined with carbothermal reduction method. Benefiting from the high-speed three-dimensional pathway for electron transport provided by the in-situ formed botryoidal highly conductive network, the Li 2 S@C/CNT cathode exhibits ultrahigh initial discharge capacity (1028.5 mA h g − 1 @1 C), superior cycle stability (520.6 mA h g − 1 after 200 cycles), and remarkable rate capability (301.8 mA h g − 1 @5 C). This work not only presents a simple and feasible approach for the low-cost preparation of high‑performance Li 2 S cathode, but also proposes an innovative idea for advancing the development of high energy density lithium–sulfur batteries.

研究领域: 材料科学 · 能源存储
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Promoting the conversion of Li2S by functional additives phenyl diselenide in Lithium–Sulfur batteries

Xueya Zhang,Jie Li,Chunhui Gao,Chenyang Shi,Liang He,Qian Xiang,Bo Hong,Yanqing Lai,Zhian Zhang,Kai Zhang

Lithium–Sulfur (Li–S) battery is a promising device in the field of electrochemical energy storage since its high specific capacity and low cost. However, the low insoluble Li 2 S conversion efficiency and uncontrollable deposition on the electrodes lead to low sulfur utilization, poor reversibility and rapid capacity decay. Consequently, the practical application of Li–S battery is limited. Herein, phenyl diselenide (PDSe) is added into the conventional electrolyte try to improve the batteries performance. The results show that the Se–Se bond in PDSe is broken and the Li–S bond in Li 2 S is elongated induced by PDSe. Moreover, PDSe promotes Li 2 S conversion and reduces Li 2 S deposition on the electrodes. As a result, the batteries using the electrolyte with PDSe exhibit enhanced discharge capacity and improved rate performance. Particularly, the batteries with 5.0 wt% PDSe additive exhibit a high initial discharge capacity of 1585.6 mAh g −1 , even after 300 cycles at 0.5 C, the batteries still maintain 916.5 mAh g −1 , which is much higher than conventional batteries of 618.7 mA h g −1 .

研究领域: 材料科学 · 电化学
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