Energy Storage Materials
·
2023
·
IF 20.4
Lihan Chen,Xianzhun Huang,Ruotong Ma,Wenyi Xiang,Jian Ma,Yueyue Wu,Ding Yang,Chengwei Wang,Weiwei Ping,Hongfa Xiang
Composite solid-state electrolytes (SSEs) can improve the flexibility of the oxide SSEs to decrease the interfacial resistance between the electrolytes and the electrodes. However, the ceramic nanofillers within the composite SSEs suffer from the agglomeration at high concentrations, decreasing the ion conductivities. In this study, a continuous nanocrystal Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZTO) skeleton is prepared by the ultrafast high-temperature sintering (UHS) together with tape-casting. Due to the short sintering time of ∼5 s from precursors, the LLZTO grains are restrained to ∼300 nm with limited Li loss. Even with trace solvent (3 wt%), the composite SSE membrane exhibits an ion conductivity of 5 × 10 −4 S⋅cm −1 , ∼50 times higher than the DOL electrolyte (1 × 10 −5 S⋅cm −1 , 8 wt% solvent), which further proves the high Li-ion conductivity of the nanocrystal LLZTO skeleton. The composite SSE membrane exhibits a critical current density of 3.4 mA⋅cm −2 , among the highest reported values for ceramic-polymer SSEs. The Li/composite SSEs/Li symmetric cells can cycle ∼ 120 h at the current density from 0.2 to 0.4 mA⋅cm −2 . The LiFePO 4 /LLZTO-PEGDA composite SSEs/Li full cell exhibits a high specific discharge capacity of ∼150 mAh⋅g −1 for ∼50 cycles with a Coulombic efficiency of ∼97%. To explore the processability of the membrane with large size, we also demonstrate a pouch cell (2 cm × 5 cm) with a high specific capacity of ∼150 mAh⋅g −1 for ∼25 cycles and a capacity retention of ∼94.5%. This work paves a new way to manufacture the nanocrystal ceramic SSE skeleton for high energy density all-solid-state batteries.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·Vol. 26
·期 12
·7231-7245
·
IF 9.3
Yutao Yang,Rongzheng Tian,Hongzhou Zhang,Zhenyu Wang,Lianqi Zhang,Yongan Yang,Dawei Song
Lithium sulfide (Li2S) is the critical raw material used for the synthesis of sulfide solid-state electrolytes, but its high cost and pollution restrict the commercialization of sulfide solid-state electrolytes and sulfide-based all-solid-state batteries. A new green and cost-effective method for the synthesis of high-quality Li2S is designed and proposed in this work. The method of reducing Li2SO4 with H2 circumvents the disadvantages of many side reactions, complicated purification processes, impure products and emission of greenhouse gases (CO and CO2) associated with traditional carbothermal reduction methods, and high-purity Li2S (H-Li2S) is obtained. Subsequently, H-Li5.6PS4.6Cl1.4 solid electrolyte was synthesized and compared with the C-Li5.6PS4.6Cl1.4 electrolyte synthesized from commercial Li2S (C-Li2S). The ionic conductivity (8.06 mS cm−1) and chemical/electrochemical stability as cathode/anode material were better than those of C-Li5.6PS4.6Cl1.4. Besides, the rate performance and long cycling stability of an all-solid-state lithium battery NCM//Li5.6PS4.6Cl1.4//Li–In assembled with H-Li5.6PS4.6Cl1.4 are better than those of batteries assembled with C-Li5.6PS4.6Cl1.4. It can maintain a discharge capacity of 133.23 mA h g−1 after 300 cycles at 1C (95% of the initial discharge capacity), and has a high discharge capacity of 127.9 mA h g−1 at 3C. The high electrochemical performance of the all-solid-state battery confirms the superiority of high-purity H-Li2S and the advantages of the hydrogen reduction method.
研究领域:
材料科学
·
电化学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Feng Sun,Zhihui Ma,Shenghai Xin,Yidi Fu,Ping Li,Jianbin Li,Qi Wan,Xuanhui Qu
Silicon (Si) anode is a promising anode material for all-solid-state lithium batteries with ultra-high theoretical specific capacity and low lithium dendrite risk. However, the inevitable vast volume expansion of Si anode during charge/discharge is recognized as a major limitation preventing its commercial application. Herein, an N, S self-doped amorphous carbon layer coated on porous micron-sized Si (p-mSi@C) is designed to construct an electron/ion conducting network while ensuring structural and interfacial stability. Uneven distribution of von mises stresses during p-mSi lithiation leads to irregular volume expansion and even fragmentation. Meanwhile, the growth of by-products at the interface between p-mSi and electrolyte contact leads to a rapid capacity decay. Compared to p-mSi anode, p-mSi@C reduces the risk of fragmentation thanks to the stress-absorbing effect of amorphous carbon, delivering excellent electrochemical performance (2679.65 mAh g −1 at 0.2 mA cm −2 with initial coulombic efficiency of 84%). More importantly, the chemical failure mechanisms of p-mSi and p-mSi@C composite anodes are revealed through structural characterization, chemical analysis, and simulation, which provides the necessary theoretical guidance for practicalization.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Wei Liu,Qiao Wang,Quan Ouyang,Xin Zhang,Yaowen Wang,Haitong Tang,Tianmin He,Chuang Yu,Guangshe Li,Liping Li
Na 3 Zr 2 Si 2 PO 12 (NZSP) shows great potential as candidate of solid electrolyte for solid-state sodium batteries. Herein, a high density NZSP solid electrolyte with space group of C2/c is synthesized by a new strategy. Such new strategy rivets most of NaF at the grain boundaries, effectively increasing the density of NZSP pellets. A small amount of F - doped into the lattice alters the lattice parameters of NZSP. The riveted NaF and doped F - cooperatively enhance the ionic conductivity of NZSP solid electrolyte. The optimized NZSP solid electrolyte, containing 3 wt%NaF additives and sintered at 1050 °C, exhibits a room-temperature Na + conductivity of 7.2×10 −4 S cm −1 and low activation energy of 0.23 eV. The solid-state battery using the optimized sample NZSP+3 wt%NaF as solid electrolyte has a wide electrochemical window of up to 7.0 V ( vs . Na + /Na) and ultra-stable cycling capability towards the bare sodium metal. The corresponding symmetrical battery demonstrates stable and reversible cycle at 0.2 mA cm −2 for 700 h with negligible voltage polarization, the longest cycling time reported to date at this current density. At current density of 0.08 mA cm −2 (0.5 C), all-solid-state battery of Na 3 V 2 (PO 4 ) 3 /NZSP+3 wt%NaF/Na can deliver a discharge capacity of 62 mAh g −1 after 60 cycles. The interfacial rivet method offers valuable insights and inspiration for the development of other types of ceramic solid electrolytes.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACTA MATERIALIA
·
2025
·
IF 9.3
Yuting Huang,Shenghao Jing,Huaqing Shen,Sijia Li,YuXin Shen,Yuanyuan Lin,Ying Zhang,Zongliang Zhang,Yang Liu,Yongle Chen,Fangyang Liu,Yang Lu
Silicon anode is one of the most promising anode materials for sulfide all-solid-state batteries (ASSBs) due to its high theoretical specific capacity of up to 4200 mAh g −1 . However, raw silicon anodes suffer from their intrinsic limitations, including low ionic and electronic conductivity, as well as significant mechanical stress arising from large volume changes during cycling. These factors contribute to the poor cycle life of silicon-based ASSBs. Herein, a double-layer structure composed of lithium-rich Li 4.4 Si alloy layer and nano silicon (nSi) anode layer, is proposed to address these issues. The double-layer structure enriches Li 4.4 Si on the current collector side, serving as conductive lithium reservoir that improves the Li + transport and electron conductivity. The low elastic modulus of Li 4.4 Si alleviates the mechanical stress induced by volume changes in the silicon upper layer. Finite element analysis indicates that the double-layer design reduces interfacial stress by three times, ensuring effective interfacial contact and providing abundant Li⁺ transport pathways. The ASSBs employing the double layer silicon anode coupled with LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811) cathode exhibit exceptional cycle stability, achieving the capacity retention rate of 86.50 % after 200 cycles at 0.5 C. Furthermore, a remarkable cell-level energy density of 308.04 Wh kg −1 was achieved at a high loading of 3.38 mAh cm −2 . The double-layer Li 4.4 Si/nSi anode can be incorporated into pouch cells, demonstrating good cycling stability. This design holds significant potential for the transition of sulfide ASSBs from laboratory-scale development to industrial applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2025
·Vol. 36
·期 12
·1-14
·
IF 2.8
Mei Rui,Yan Feng,Hu Sizheng,Gong Zonggui,Guo Haoxuan,Wang Qijing,Zheng Xinghua
With the increasingly urgent safety requirement of lithium-ion batteries, more and more attention has been paid to Li 7 La 3 Zr 2 O 12 (LLZO)-based solid electrolytes with high ion conductivity and excellent electrochemical performance. Unfortunately, owing to the serious “Li-loss” and the abnormal grain growth (AGG) during the long-time high-temperature sintering process, it is difficult to achieve the high-quality LLZO electrolyte with uniform and fine grains, high density and excellent electrochemical performance. In this work, Ga/Mo co-doped LLZO solid-state electrolytes have been prepared by traditional sintering (TS) and two-step sintering (TSS). And the sintering mechanism, phase stability, microstructure evolution, and electrochemical performance have been systematically investigated. A small amount of Ga/Mo doping not only promotes the formation of the cubic garnet LLZO phase, but also enhances the stability of cubic phase. High density of 92.3% and uniform microstructure without AGG have been achieved via a small amount of Ga doping and TSS. Li 6.3 Ga 0.1 La 3 Zr 1.8 Mo 0.2 O 12 electrolytes, prepared by TSS of 1200 °C/15 min-1100 °C/8 h, exhibits high ion conductivity of 2.59 × 10 –4 S·cm −1 and critical current density (CCD) value of 0.5 mA·cm −2 , low electric conductivities of 4.77 × 10 –9 S·cm −1 , which suggests it is a potential electrolyte to apply in all-solid-state batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
COMPOSITES SCIENCE AND TECHNOLOGY
·
2019
·
IF 6.309
Xuelian Fu,Yuchao Li,Chengzhu Liao,Weiping Gong,Mingyang Yang,Robert Kwok Yiu Li,Sie Chin Tjong,Zhouguang Lu
Low ionic conductivity and large interfacial impedance between the electrode and electrolyte are the main bottleneck issues of the current solid electrolytes . In this study, a novel 3D hierarchical solid electrolyte was developed to tackle the large interfacial impedance problem. A flexible polyethylene oxide/lithium chlorate (PEO/LiClO 4 ) was in-situ formed inside the 3D porous Li 6.28 La 3 Zr 2 Al 0.24 O 12 (LLZAO) network by simply using a cleanroom wiper as the template. The obtained 3D LLZAO-PEO/LiClO 4 composite solid electrolyte exhibited a high ionic conductivity of 2.25 × 10 −5 S cm −1 at 30 °C, being 30.7 times higher than that of pristine PEO/LiClO 4 electrolyte. The improved ionic conductivity was attributed to the 3D porous LLZAO structure with continuous fast ion transport pathways. In addition, the 3D LLZAO network can effectively inhibited the growth of lithium dendrite , leading to excellent stability and desirable safety during lithium stripping/plating cycling. Furthermore, the all-solid-state LiFePO 4 /Li battery system based on the obtained 3D LLZAO-PEO/LiClO 4 electrolyte showed a high initial discharge specific capacity of 143.8 mAh·g −1 and a high capacity retention of 86% after 200 cycles at 60 °C. This 3D composite solid electrolyte design is very effective in reducing the interfacial impedance and provides a solution for the further development of high-performance solid electrolyte for all-solid-state rechargeable batteries.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
Advanced Science
·
2023
·Vol. 10
·期 32
·2302618
·
IF 15.1
Wei Zhou,Changsheng Song,Shuyang Li,Miao Liu,Huiwen He,Shaoyu Yang,Jin Xie,Fei Wang,Fang Fang,Dalin Sun,Jie Zhao,Yun Song
All-solid-state sodium-ion batteries have the potential to improve safety and mitigate the cost bottlenecks of the current lithium-ion battery system if a high-performance electrolyte with cost advantages can be easily synthesized. In this study, a one-step dehydrogenation-assisted strategy to synthesize the novel thio-borohydride (Na-B-H-S) electrolyte is proposed, in which both raw material cost and preparation temperature are significantly reduced. By using sodium borohydride (NaBH 4 ) instead of B as a starting material, B atoms can be readily released from NaBH 4 with much less energy and thus became more available to generate thio-borohydride. The synthesized Na-B-H-S (NaBH 4 /Na-B-S) electrolyte exhibits excellent compatibility with current cathode materials, including FeF 3 (1.0–4.5 V), Na 3 V 2 (PO 4 ) 3 (2.0–4.0 V), and S (1.2–2.8 V). This novel Na-B-H-S electrolyte will take a place in mainstream electrolytes because of its advantages in preparation, cost, and compatibility with various cathode materials.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Jun Zhang,Haoyue Zhong,Chao Zheng,Yang Xia,Chu Liang,Hui Huang,Yongping Gan,Xinyong Tao,Wenkui Zhang
The synthesis of solid electrolytes with high ionic conductivity and the design of electrode interface with preferable compatibility are critical to realize the bulk-type application of all-solid-state batteries. In order to realize the superior electrochemical performance, argyrodite Li 6 PS 5 Cl is a promising solid electrolyte in all-solid-state batteries due to high ionic conductivity and electrochemical stability. Meanwhile, the solution reprecipitation is a valid process providing intimate ionic contact between electrodes and electrolytes to mitigate the interface incompatibility. Here, a wet-slurry process by dispersing active material (LiNi 0.8 Co 0.1 Mn 0.1 O 2 ), solid electrolyte (Li 6 PS 5 Cl), binder (ethyl cellulose) and conductive additives (carbon black) in anhydrous ethanol is developed to fabricate cathode. The effect of different contents of the binder in the composite cathodes on the electrochemical performance is investigated. The all-solid-state battery with a composite cathode containing 1 wt% of ethyl cellulose shows a reversible discharge capacity of 111.7 mAh g −1 at 30 °C and its capacity retention is approximately 89.7% after 100 cycles. This work demonstrates that the fast ion migration and stable interface between active particles and solid electrolyte enabled by optimum content of chemically compatible binder are critical to the electrochemical performance of all-solid-state lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态离子学
·
锂离子电池
·
纳米复合材料
·
界面工程
✓ 已验证
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 33
·2301275
·
IF 13.3
Huaxin Liu,Laiqiang Xu,Hanyu Tu,Zheng Luo,Fangjun Zhu,Wentao Deng,Guoqiang Zou,Hongshuai Hou,Xiaobo Ji
Solid-state polymer electrolytes are highly anticipated for next generation lithium ion batteries with enhanced safety and energy density. However, a major disadvantage of polymer electrolytes is their low ionic conductivity at room temperature. In order to enhance the ionic conductivity, here, graphene quantum dots (GQDs) are employed to improve the poly (ethylene oxide) (PEO) based electrolyte. Owing to the increased amorphous areas of PEO and mobility of Li + , GQDs modified composite polymer electrolytes achieved high ionic conductivity and favorable lithium ion transference numbers. Significantly, the abundant hydroxyl groups and amino groups originated from GQDs can serve as Lewis base sites and interact with lithium ions, thus promoting the dissociation of lithium salts and providing more ion pathways. Moreover, lithium dendrite is suppressed, associated with high transference number, enhanced mechanical properties and steady interface stability. It is further observed that all solid-state lithium batteries assembled with GQDs modified composite polymer electrolytes display excellent rate performance and cycling stability.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Qiyue Luo,Chuang Yu,Chaochao Wei,Shuai Chen,Shaoqing Chen,Ziling Jiang,Linfeng Peng,Shijie Cheng,Jia Xie
Li 10 GeP 2 S 12 shows great potential as solid electrolytes for solid-state batteries due to its ultrahigh Li-ion conductivity. However, the high cost of Ge and the poor stability limit its applications. Replacing Ge with Sn can significantly lower the cost and maintains the high conductivity, while the corresponding Li 10 SnP 2 S 12 still suffers the low interfacial stability with the bare high voltage layered oxide cathodes. Herein, Li 10 SnP 2 S 12 with high Li-ion conductivity up to 4.79 mS cm −1 has been synthesized. All-solid-state battery using the cathode consisting of bare LiNi 0.6 Co 0.2 Mn 0.2 O 2 and Li 10 SnP 2 S 12 shows low capacities and poor cyclability due to side reactions between those two particles. To improve the interfacial stability, a highly conductive Li 3 InCl 6 electrolyte is introduced both in the cathode mixture and between the cathode layer and Li 10 SnP 2 S 12 solid electrolyte layer. This new configuration delivers superior electrochemical performances at different operating temperatures. It delivers high initial discharge capacities of 176.1 mAh g −1 , 186.9 mAh g −1 , and 73.7 mAh g −1 at 0.1C when operated at room temperature, 60 o C, and −20 o C, respectively. The superior battery performances are attributed to the excellent electrochemical stability of Li 3 InCl 6 electrolyte towards bare LiNi 0.6 Co 0.2 Mn 0.2 O 2 cathode. This work provides a guideline to design Li 10 SnP 2 S 12 -based all-solid-state lithium batteries with high energy density and long span life.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Qiyue Luo,Siwu Li,Chaochao Wei,Zhongkai Wu,Chen Liu,Ziling Jiang,Lin Li,Shaoqing Chen,Chuang Yu
Sulfide-based all-solid-state batteries are currently a focal point of research for next-generation energy storage solutions. However, the poor antioxidative stability of sulfide electrolytes limits their practical applications. In this study, we strengthen sulfur-related bonding interactions by regulating the local charge density of the surrounding sulfur atoms, thereby enhancing the oxidative stability of sulfide electrolytes. First-principles calculations and experimental results demonstrate that substituting certain sulfur in Li9.9SnP2S11.9Br0.1 with oxygen leads to an increase in the local electronic density around unsubstituted sulfur atoms and a reduction in cation–anion bond lengths, which subsequently strengthens the bonds including P–S and Sn–S. Remarkably, the tailored electrolyte also exhibits significant improvements in air stability and chemical compatibility with halide electrolytes. Batteries constructed with the obtained Li9.9SnP2S10.9Br0.1O1.0 electrolyte demonstrated greatly enhanced electrochemical performance. Our results highlight how local charge distribution regulation enhances the chemical and electrochemical stability of sulfide electrolytes, offering valuable insights for creating high-performance all-solid-state batteries.
研究领域:
材料科学
·
能源存储
·
固体物理
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）