ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Aiguo Han,Rongzheng Tian,Liran Fang,Fengming Wan,Xiaohu Hu,Zixiang Zhao,Fangyuan Tu,Dawei Song,Xin Zhang,Yongan Yang
Li6PS5Cl is an extensively studied sulfide-solid-electrolyte for developing all-solid-state lithium batteries. However, its practical application is hindered by the high cost of its raw material lithium sulfide (Li2S), the difficulty in its massive production, and its substandard performance. Herein we report an economically viable and scalable method, denoted as “de novo liquid phase method”, which enables in synthesizing high-performance Li6PS5Cl without using commercial Li2S but instead in situ making Li2S from cheap materials of lithium chloride (LiCl) and sodium sulfide. LiCl, a raw material needed for making both Li2S and Li6PS5Cl, can be added at a full-scale in the beginning and unrequired to separate when making the intermediate Li3PS4. Such a consecutive feature makes this method time-efficient; and the excess amount of LiCl in the step of making Li2S also facilitates removing the byproduct of sodium chloride via the common ion effect. The materials cost of this method for Li6PS5Cl is ∼ $55/kg, comparable with the practical need of $50/kg. Moreover, the obtained Li6PS5Cl shows high ionic conductivity and outstanding cyclability in full battery tests, that is, ∼2 mS/cm and >99.8% retention for 400+ cycles at 1 C, respectively. Thus, this innovative method is expected to pave the way to develop practical sulfide-solid-electrolytes for all-solid-state lithium batteries.
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
Results in Chemistry
·
2022
·
IF 0
Chenguang Zhao,Miaomiao Lyu,Chuangji Bi,Sida Huo,Sirui Li,Wendong Xue
Argyrodite-type solid electrolyte have attracted great attention due to its high ionic conductivity and stability to lithium anode. In this experiment, argyrodite-type Li 6 PS 5 Cl was prepared by the solid-state method. The Li 6 PS 5 Cl solid electrolyte prepared by the solid-state sintering process has more pore and defects, resulting in lower ion conductivity of the electrolyte. The highest ionic conductivity was only 9.58 × 10 −4 S cm −1 . In order to decrease the defects in the Li 6 PS 5 Cl, a new type of second sintering process is used. The highest ionic conductivity obtained by this new process was up to 3.19 × 10 −3 S cm −1 , which was a relatively high value in currently reported. Industrial Computed Tomography (CT) technology was an advanced characterization method to observe the quantity, size, and distribution of defects inside the sample without any damage. In this experiment, industrial CT was used to detect the pores in Li 6 PS 5 Cl., finding that the second sintering process successfully reduces the quantity and size of pores in Li 6 PS 5 Cl solid electrolyte, uniforming the distribution of pores thus improving the ion conductivity of the Li 6 PS 5 Cl solid electrolyte. This new preparation and characterization method might provide a new idea for the further research of Li 6 PS 5 Cl.
研究领域:
材料科学
·
电化学
·
固态电池
✓ 已验证
DOI
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 31
·18612-18618
·
IF 10.733
Shuo Wang,Xiaofu Xu,Xue Zhang,Chengzhou Xin,Bingqing Xu,Liangliang Li,Yuan-Hua Lin,Yang Shen,Baohua Li,Ce-Wen Nan
All-solid-state lithium-ion batteries (ASSLIBs) owing to their advantage of enhanced safety are considered to be a promising candidate for next-generation energy storage devices. However, the poor cycling performance and low areal capacities of ASSLIBs with S, Li2S or traditional oxide cathodes hinder the development of high-energy-density ASSLIBs. Herein, a Li6PS5Cl solid-state electrolyte has been systematically investigated for use as a cathode active material in ASSLIBs for the first time. ASSLIBs employing Li6PS5Cl as both the active material and electrolyte with a Li–In alloy anode are fabricated. A Li6PS5Cl-based cell with an active material loading of 3.1 mg cm−2 exhibits a high discharge capacity of around 535 mA h g−1 after 650 cycles at 56 mA g−1 (∼0.1C) at room temperature, which is the highest value among ASSLIBs using sulfide SSEs as active materials and is even comparable with those of cells with S, Li2S or transition metal sulfides as the active material. This superior long-term cycling performance is attributed to the highly reversible electrochemical activity of Li6PS5Cl revealed by ex situ XRD and XPS analyses.
研究领域:
电化学
·
能源材料
·
固态离子学
·
储能技术
·
材料科学
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 15
·2310356
·
IF 27.4
Shijie Xu,Xiaobin Cheng,Shunjin Yang,Yichen Yin,Xinyu Wang,Yuzhe Zhang,Dehang Ren,Yujiang Sun,Xiao Sun,Hongbin Yao,Yongan Yang
Li 6 PS 5 Cl (LPSC) is a very attractive sulfide solid electrolyte for developing high-performance all-solid-state lithium batteries. However, it cannot suppress the growth of lithium dendrites and then can only tolerate a small critical current density (CCD) before getting short-circuited to death. Learning from that a newly-developed LaCl 3 -based electrolyte (LTLC) can afford a very large CCD, a three-layer sandwich-structured electrolyte is designed by inserting LTLC inside LPSC. Remarkably, compared with bland LPSC, this hybrid electrolyte LPSC/LTLC/LPSC presents extraordinary performance improvements: the CCD gets increased from 0.51 to 1.52 mA cm −2 , the lifetime gets prolonged from 7 h to >500 h at the cycling current of 0.5 mA cm −2 in symmetric cells, and the cyclability gets extended from 10 cycles to >200 cycles at the cycling rate of 0.5 C and 30 °C in Li|electrolyte|NCM721 full cells. The enhancing reasons are assigned to the capability of LTLC to scavenge lithium dendrites, forming a passive layer of Ta, La, and LiCl.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
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
Chemical Science
·
2025
·Vol. 16
·期 23
·10289-10295
·
IF 7.4
Deye Sun,Wenru Li,Yantao Wang,Jiangwei Ju,Pengxian Han,Shanmu Dong,Jun Ma,Guanglei Cui
High voltage has been considered the primary factor causing electrolyte decomposition in all-solid-state lithium batteries. However, whether high voltage is the only decisive factor in sulfide electrolyte decomposition is an open question. Herein, we redefined the decomposition conditions of sulfide electrolytes under the combined effect of high voltage (≥5 V vs. Li+/Li) and large Li+ flux by recording the decomposition process of Li6PS5Cl via in situ Raman spectroscopy during cyclic voltammetry measurement. The result shows that under the combined action of high voltage and large Li+ flux, PS43− anions of Li6PS5Cl undergo much more severe deformation and decomposition than they do only at high voltage or large Li+ flux. At the same time, it also suggests that the much severe decomposition of Li6PS5Cl located near the surface of cathode particles compared to that in the bulk region of Li6PS5Cl may be the combined result of electrochemical/chemical reactions and high voltage/large Li+ flux. Furthermore, the effect of large Li+ flux on the irreversible decomposition of Li6PS5Cl supplements our understanding of the electrochemical stability of solid electrolytes. This work redefines the stability of sulfide electrolyte and gives directions to design highly stable bulk and interfacial structures of sulfide electrolytes at high voltage and high current density.
研究领域:
材料科学
·
电化学
·
固态电池
·
储能技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Bo Pang,Zhan Wu,Wenkui Zhang,Hui Huang,Yongping Gan,Yang Xia,Xinping He,Xinhui Xia,Jun Zhang
Agroydite Li 6 PS 5 Cl is one of the most promising solid electrolytes because of its high ionic conductivity and good processability. However, there are still many challenges with Li 6 PS 5 Cl and lithium anodes that prevent their industrialization, such as the growth of lithium dendrite and interfacial reactions. Interface modification of anodes has proven to be an effective method for solving these problems. Herein, we introduce Ag nanoparticles into the interface between Li 6 PS 5 Cl and metallic lithium and systematically investigate their interfacial properties . By incorporating silver nanoparticles , lithium dendrites can be depleted by forming Li–Ag alloys. Therefore, a denser and more stable interface between Li 6 PS 5 Cl and lithium metals is obtained. Benefiting from the above advantages, the Li/Li symmetrical battery with incorporated Ag nanoparticles exhibited an ultrahigh critical current density of up to 10 mA cm −2 and great cycling stability (more than 600 h). An all-solid-state battery with Ni-rich cathode and lithium metal anode demonstrates a high-capacity retention rate of 84% after 200 cycles at a current density of 0.5C. This study provides new insights into the construction of stable anode interfaces for the practical application of all-solid-state lithium batteries.
研究领域:
材料科学
·
电化学
·
固态离子学
·
能源材料
·
电池技术
·
界面工程
✓ 已验证
DOI
高影响因子
Gels
·
2024
·Vol. 10
·期 3
·199
·
IF 5
Xinghua Liang,Xueli Shi,Lingxiao Lan,Yunmei Qing,Bing Zhang,Zhijie Fang,Yujiang Wang
Gel electrolytes for lithium-ion batteries continue to replace the organic liquid electrolytes in conventional batteries due to their advantages of being less prone to leakage and non-explosive and possessing a high modulus of elasticity. However, the development of gel electrolytes has been hindered by their generally low ionic conductivity at room temperature and high interfacial impedance with electrodes. In this paper, a poly (vinylidene fluoride)-hexafluoropropylene copolymer (PVdF-HFP) with a flexible structure, Li6PS5Cl (LPSCl) powder of the sulfur–silver–germanium ore type, and lithium perchlorate salt (LiClO4) were prepared into sulfide gel composite electrolyte films (GCEs) via a thermosetting process. The experimental results showed that the gel composite electrolyte with 1% LPSCl in the PVdF-HFP matrix exhibited an ionic conductivity as high as 1.27 × 10−3S·cm−1at 25 °C and a lithium ion transference number of 0.63. The assembled LiFePO4||GCEs||Li batteries have excellent rate (130 mAh·g−1at 1 C and 54 mAh·g−1at 5 C) and cycling (capacity retention was 93% after 100 cycles at 0.1 C and 80% after 150 cycles at 0.2 C) performance. This work provides new methods and strategies for the design and fabrication of solid-state batteries with high ionic conductivity and high specific energy.
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
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2024
·Vol. 30
·期 3
·250-261
·
IF 6.7
Cao Xiaorou,Xu Shijie,Zhang Yuzhe,Hu Xiaohu,Yan Yifan,Wang Yanru,Qian Haoran,Wang Jiakai,Chang Haolong,Cheng Fangyi,Yang Yongan
All-solid-state lithium-metal batteries (ASSLMBs) are widely considered as the ultimately advanced lithium batteries owing to their improved energy density and enhanced safety features. Among various solid electrolytes, sulfide solid electrolyte (SSE) Li 6 PS 5 Cl has garnered significant attention. However, its application is limited by its poor cyclability and low critical current density (CCD). In this study, we introduce a novel approach to enhance the performance of Li 6 PS 5 Cl by doping it with fluorine, using lithium fluoride nanoparticles (LiFs) as the doping precursor. The F-doped electrolyte Li 6 PS 5 Cl-0.2LiF(nano) shows a doubled CCD, from 0.5 to 1.0 mA/cm 2 without compromising the ionic conductivity; in fact, conductivity is enhanced from 2.82 to 3.30 mS/cm, contrary to the typical performance decline seen in conventionally doped Li 6 PS 5 Cl electrolytes. In symmetric Li|SSE|Li cells, the lifetime of Li 6 PS 5 Cl-0.2LiF(nano) is 4 times longer than that of Li 6 PS 5 Cl, achieving 1500 h vs. 371 h under a charging/discharging current density of 0.2 mA/cm 2 . In Li|SSE|LiNbO 3 @NCM721 full cells, which are tested under a cycling rate of 0.1 C at 30 °C, the lifetime of Li 6 PS 5 Cl-0.2LiF(nano) is four times that of Li 6 PS 5 Cl, reaching 100 cycles vs. 26 cycles. Therefore, the doping of nano-LiF offers a promising approach to developing high-performance Li 6 PS 5 Cl for ASSLMBs. Graphical Abstract
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Jun Zhang,Chao Zheng,Jiatao Lou,Yang Xia,Chu Liang,Hui Huang,Yongping Gan,Xinyong Tao,Wenkui Zhang
Argyrodite Li 6 PS 5 Cl is a promising solid electrolyte in all-solid-state lithium batteries owing to its high ionic conductivity . However, the poor mechanical property and undesirable interfacial property restrict its application. In order to solve these issues, we fabricate Li 6 PS 5 Cl/poly(ethylene oxide) composite solid electrolytes with enhanced mechanical property and stable lithium/electrolyte interface. By adding 5 to 20 wt% poly(ethylene oxide), the proportional limit of composite solid electrolytes is enhanced by ∼150%, reaching a value up to 60 MPa. With 5 wt% poly(ethylene oxide), the as-assembled sandwich-type LiNi 0 · 8 Co 0 · 1 Mn 0 · 1 O 2 /composite solid electrolytes/Li battery exhibits enhanced cycling performance with a capacity retention rate of 91% over 200 cycles at 0.05C and 30 °C. Ex situ characterizations reveal that by adding suitable poly(ethylene oxide) content in Li 6 PS 5 Cl, the interfacial reactions and lithium dendrite growth can be effectively inhibited, resulting in much improved cycling performance of all-solid-state lithium batteries.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Changfei Zou,Li Yang,Kaili Luo,Lei Liu,Xiyuan Tao,Lingguang Yi,Xianhu Liu,Xiaoyan Zhang,Xianyou Wang
Due to the advantages of high safety and high energy density, solid-state lithium batteries (SSLBs) are promising competitors for next-generation batteries. Unfortunately, the growth of Li dendrites and irreversible capacity loss caused by the Li metal anode/solid electrolyte interfacial incompatibility remain challenges. Herein, an in situ formed artificial protective layer between the lithium metal anode and solid electrolyte Li6PS5Cl (LPSC) is introduced. A stable solid electrolyte interface (SEI) is in situ formed in the Li/Li6PS5Cl interface via the electrochemical reduction of the liquid electrolyte LiTFSI/tetraethylene glycol dimethyl ether (Li(G4)TFSI), which is beneficial for the improvement of the stability of interfacial chemistry and homogeneous lithium deposition behavior. The assembled Li/Li(G4)TFSI-assisted Li6PS5Cl/Li symmetric cells enable stable cycles for 850 and 400 h at a current density of 0.1 and 0.2 mA/cm2, respectively. Moreover, the LiNi0.6Co0.1Mn0.3O2(NCM613)/Li(G4)TFSI-assisted Li6PS5Cl/Li SSLBs can achieve prominent cycling stability at room temperature. This work provides a new insight into the interfacial modification to design SSLBs with high energy density.
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 Energy Materials
·
2022
·Vol. 12
·期 25
·2200660
·
IF 29.698
Sijie Liu,Le Zhou,Jian Han,Kaihua Wen,Shundong Guan,Chuanjiao Xue,Zheng Zhang,Ben Xu,Yuanhua Lin,Yang Shen,Liangliang Li,Ce-Wen Nan
All-solid-state batteries (ASSBs) using sulfide electrolytes have attracted ever-increasing interest due to high ionic conductivity of the sulfides. Nevertheless, a thin, strong solid-state sulfide electrolyte membrane maintaining high ionic conductivity is highly desired for ASSBs. Here, a thin, flexible composite solid electrolyte membrane composed of argyrodite sulfide Li 6 PS 5 Cl and a polar poly(vinylidene fluoride- co -trifluoroethylene) (P(VDF-TrFE)) framework is prepared via an electrospinning-infiltration-hot-pressing method. The interaction between Li 6 PS 5 Cl and polar P(VDF-TrFE) ensures a high lithium-ion conductivity (≈1.2 mS cm –1 ) at room temperature and good mechanical ductility of the composite electrolyte membrane. The coin-type ASSB cells with the thin composite electrolyte membrane, a composite cathode of LiNbO 3 -coated LiNi 0.8 Co 0.1 Mn 0.1 O 2 and Li 6 PS 5 Cl, and a lithium-indium anode, show super cycling performance, and the capacity retention is 92% after 1000 cycles and 71% even after 20 000 cycles at 1.0 mA cm –2 (i.e., 1.61 C) at room temperature. Moreover, pouch-type ASSB cells with a high mass loading of active materials are made to demonstrate the potential and feasibility in future commercial applications.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态离子学
·
纳米材料
·
电池技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）