JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Qingya Guo,Fanglin Xu,Lin Shen,Zhiyan Wang,Jia Wang,Hao He,Xiayin Yao
Polyethylene oxide (PEO)/Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) composite solid electrolyte is considered as a promising electrolyte for lithium batteries . However, LLZTO nanoparticles tend to agglomerate in PEO/LLZTO composite polymer electrolyte due to interfacial incompatibility between PEO and LLZTO nanoparticles , which leads to low ionic conductivity , poor interface stability with the electrode, and inferior batteries cycling stability. In order to enhance interfacial compatibility, herein, LLZTO nanoparticles are modified through firstly surface-functionalizing by dopamine coating and then grafting poly (ethylene glycol) (PEG) brush on it via amino and epoxy reaction. As a consequence, the ionic conductivity of LLZTO/PEO composite polymer electrolyte filled with 2 wt% modified LLZTO increases up to 1.1 × 10 − 4 S cm −1 , which is about twice and 20 times in comparison with LLZTO/PEO filled with 2 wt% unmodified LLZTO and PEO electrolytes, respectively. Moreover, high oxidation potential of around 4.8 V and ionic transference number of 0.34 as well as good interface stability with lithium anode are also achieved. Thus, LiFePO 4 ||Li all-solid-state lithium metal batteries based on LLZTO/PEO composite polymer electrolyte filled with 2 wt% modified LLZTO exhibit excellent cyclic stability of 152.3 mAh g −1 with capacity retention of 90.35% at 0.5 C after 500 cycles under 60 °C.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Pengyuan Dong,Qiang Deng,Qimeng Zhang,Changdong Chen,Chenghao Yang
The garnet-type solid electrolyte Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) was modified with a cationic surfactant Cetyltrimethylammonium Bromide (CTAB) to improve the dispersion of LLZTO inorganic particles in Poly (ethylene oxide) (PEO) electrolyte (PEO-LLZTO@CTAB) by a liquid phase casting method. During fabrication, the cationic modifier CTAB is uniformly adsorbed on the surface of LLZTO particles, which can effectively reduce their surface energy and lead to a thin CTAB surface coating layer. This fabricated PEO-LLZTO@CTAB can avoid the aggregation of LLZTO particles in the composite solid-state electrolyte (CSSE) and improve the interfacial contact at the PEO/LLZTO interface, thus reducing the overall resistance of PEO-LLZTO@CTAB/Li half-cell and inhibiting the dendrite growth during cycling. The all-solid-state batteries (ASSBs) with LiFePO 4 (LFP) as the cathode, PEO-LLZTO@CTAB as the electrolyte and Li as the anode exhibit a high initial discharge capacity of 146.6 mAh-g −1 , excellent rate performance and high-capacity retention of 91.0 % after 300 cycles at 0.2 C multiplier and 60 °C within the voltage range of 2.7–4.0 V.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Xiaorong Zhang,Yuxue Sun,Chunhui Ma,Nan Guo,Haiyang Fan,Jun Liu,Haiming Xie
The demand for lithium-ion batteries with high safety and high energy density is leading a research boom in solid electrolytes . Composite solid electrolytes (CSEs), which combine the advantages of inorganic solid electrolytes and polymer electrolytes , have recently been intensively investigated. Herein, a novel CSE is fabricated by incorporating Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) nanoparticles into a polystyrene-poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide)-polystyrene (PS-PEO-PPO-PEO-PS) pentablock copolymer matrix. The addition of LLZTO not only improves the ionic conductivity of the CSE by reducing the degree of crystallinity of PS-PEO-PPO-PEO-PS, but also provides an additional transport channel for lithium-ions. As a result, the CSE with an optimal LLZTO content of 30 wt% shows an ionic conductivity of 3.10 × 10 −4 S cm −1 (28 °C). In addition, the CSE exhibits an electrochemical stability window of 5.1 V and a lithium ion transfer number of 0.36 at 28 °C. The low interfacial impedance indicates the formation of a stable interface between the CSE and the electrodes. Thus, LiFePO 4 /Li cells prepared using the CSE deliver high discharge capacity of 151.2 mA h g −1 with capacity retention of 95.7% after 160 cycles at 0.1C. These results demonstrate the promise of the combination of block copolymer/lithium garnet composite electrolytes for practical applications in solid lithium-ion batteries.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
IONICS
·
2021
·Vol. 27
·期 8
·3339-3346
·
IF 2.817
Liu Huirong,Li Jianling,Feng Wei,Han Guimei
Commercial lithium-ion batteries have safety risks due to the use of electrolyte-containing flammable organic solvents. The development of all solid-state lithium ion batteries with solid electrolyte is a feasible technical way to improve the safety of batteries. In this work, PVDF-based composite solid-state electrolytes (CSEs) were prepared by coupling Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) and polyvinylidene fluoride (PVDF). The electrochemical performance and interfacial compatibility between composite electrolyte and electrode were improved by the combination of appropriate amount of Li-ion-conducting particles and the insulating polymer. The corresponding solid-state battery of LiFePO 4 |PVDF-LLZTO-CSE| Li is fabricated and delivers initial discharge capacity of 162.4 mAh g -1 , and coulomb efficiency is approximately 98.5%. And the solid-state battery exhibits satisfactory rate capability and cycling stability at room temperature. This study suggests that a combination of the lithium garnet particles and insulating polymer is one of the promising methods to solve the problem of liquid electrolyte.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态离子学
·
电池技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Ran Wei,Yue Zhang,Jiameng Yu,Xinshui Zhang,Yining Zhang,Tianyi Gao,Yi Yu,Jie Zhao,Wei Liu
Ta-doped Li6.4La3Zr1.4Ta0.6O12 (LLZTO) for solid-state lithium batteries demonstrates encouraging performance; however, they encounter issues with lithium dendrite formation that impede their widespread use. Herein, we design a LLZTO ceramic with an interlayer containing a mixed dense layer of Ag and LLZTO, prepared by one-step sintering. The Ag-rich interlayer in LLZTO can hinder the growth and the penetration of lithium dendrites though the reaction between Ag and lithium metal. Compared with the Ag-free counterpart, a higher critical current density of 0.6 mA cm–2, in addition to a longer life span under a current density of 0.2 mA cm–2, is achieved by adopting the interlayer in LLZTO. This research offers novel insights into the engineering of garnet-based solid electrolytes, tailored for the advancement of high-rate lithium metal batteries.
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
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Chao Gao,Xinping Li,Guijuan Wei,Shoujuan Wang,Xixia Zhao,Fangong Kong
Solid polymer electrolytes (SPEs) have sparked attention due to their superior mechanical robustness and excellent security in solid-state lithium batteries. However, intrinsic limitations, such as poor ionic transport properties and large interface impedance, severely hinder their practical applications. Herein, a novel composite solid electrolyte (PLHL-CSE) membrane, which consists of poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), hydroxypropyl methyl cellulose (HPMC), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO), was prepared by solution-casting technique. The incorporation of HPMC into PVDF-HFP-based electrolyte played crucial roles in reducing the crystallinity of PVDF-HFP, promoting the dissociation of lithium salt, and increasing the amount of mobile Li + . With synergistic effects of HPMC and LLZTO, the mechanical and electrochemical performance of PVDF-HFP-based electrolytes were greatly enhanced. The obtained PLHL-CSE membrane showed better mechanical strength (3.0 MPa), enhanced ionic conductivity (0.25 mS/cm at 25 °C), greater lithium-ion transference number (0.7), and broadened electrochemical window of 5.0 V (vs. Li + /Li) than the PVDF-HFP/LiTFSI solid polymer electrolyte (PL-SPE) membrane. After 300 cycles at 1 C, the assembled LiFePO 4 /PLHL-CSE/Li cell with PLHL-CSE membrane as the hybrid composite solid electrolyte displayed a high capacity retention (95.6%). In addition, the positive effects of HPMC and LLZTO on promoting the generation of stable SEI and the uniform lithium deposition were also confirmed by the SEM results of cycled lithium metals. These findings point to the good potential of PLHL-CSE membrane as a hybrid composite solid electrolyte for practical application in lithium 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
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yanhua Zhang,Yuhang Mei,Xinglong Gao,Yumei Xiao,Zijun Tang,Xing Xiang,Jiadong Deng
The lithium dendrite problem of Li 7 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid electrolyte restricts the practical application and development of all-solid-state lithium batteries (ASSLBs). Herein, a LiPON interlayer with Li + conductive and electron non-conductive dynamic properties is constructed at the Li/LLZTO interface. Results show that the electronic conductivity of solid electrolyte after LiPON modification decreased by nearly three orders of magnitude, indicating that it has good ability to hinder electron conduction . The interlayer enhances the wettability between the Li metal anode and LLZTO, resulting in a decrease of battery resistance from 3400 Ω to 700 Ω. The critical current density of the ASSLBs increase from 0.1 mA cm −2 to 1.2 mA cm −2 at room temperature, and the battery cycle number increase from 31 h to over 1000 h. XPS deep etching results show that the LiPON/LLZTO interface has good electrochemical stability. The Kelvin probe force microscope displays a sharp increase in potential within the LiPON interlayer, indicating its successful hindrance of electron conduction to the solid electrolyte. The effective inhibition of lithium dendrites growth is due to LiPON can promote the Li + transmission from LLZTO solid electrolyte to Li anode, and also hinder the electron conduction to LLZTO to form lithium dendrites.
研究领域:
材料科学
·
电化学
·
能源存储
·
固态电池
·
界面工程
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Qian Zhang,Yanni Zhang,Jinyuan Zhao,Bofei Luo,Tengteng Liu,Chen Xu,Junpeng Li,Yaping Du
The garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid electrolyte is promising in the fabrication of the solid-state lithium metal battery (LMB) for its high intrinsic lithium ionic conductivity and electrochemical stability. However, the high interfacial resistance induced by the surface contamination layer and poor interfacial contact severely hinders its practical applications. Wet ball-milling in the presence of polyacrylonitrile (PAN) was found to be extremely effective in preparation for highly conductive LLZTO. The work employs four typical polymers (PMMA, PEO, PVP, and PS) in wet ball-milling jars to prepare in-situ polymer-coated LLZTO ceramic particles. Effective lithium-ion migration channels between LLZTO particles without sintering can be constructed successfully, significantly enhancing electrochemical performances. The lithium symmetric cell exhibits long-term cycling stability of over 2000 h at 65 °C and 0.1 mA cm −2 . The solid-state LMB assembled using the LiFePO 4 cathode and the solid electrolyte made from in-situ polymer-coated LLZTO particles demonstrates a discharge capacity of 120 mAh g −1 with a capacity retention of more than 95 % after 200 charge/discharge cycles at 65 °C and 0.5C. The key mechanism underlying the much-improved performance could be the in-situ formation of polymeric protective coatings on the LLZTO fresh surfaces during the wet ball-milling process. The polymer coating prevents the LLZTO from contaminating and fills the gaps between LLZTO particles, thus facilitating lithium-ion migration.
研究领域:
材料科学
·
电化学
·
储能
·
固态电池
·
高分子科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Yang Wang,Zhen Chen,Yixin Wu,Yu Li,Ziyu Yue,Minghua Chen
Lithium-ion batteries (LIBs) have achieved a triumph in the market of portable electronic devices since their commercialization in the 1990s due to their high energy density. However, safety issue originating from the flammable, volatile, and toxic organic liquid electrolytes remains a long-standing problem to be solved. Alternatively, composite solid electrolytes (CSEs) have gradually become one of the most promising candidates due to their higher safety and stable electrochemical performance. However, the uniform dispersity of ceramic filler within the polymer matrix remains to be addressed. Generally, all-solid-state lithium metal batteries without any liquid components suffer from poor interfacial contact and low ionic conductivity, which seriously affect the electrochemical performance. Here we report a CSE consisting of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), polydopamine (PDA) coated Li6.4La3Zr1.4Ta0.6O12 (LLZTO) (denoted as PDA@LLZTO) microfiller, polyacrylonitrile (PAN), and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP). Introducing only 4 μL of liquid electrolyte at the electrode|electrolyte interface, the CSE-based cells exhibit high ionic conductivity (0.4 × 10–3 S cm–1 at 25 °C), superior cycle stability, and excellent thermal stability. Even under low temperatures, the impressive electrochemical performance (78.8% of capacity retention after 400 cycles at 1 C, 0 °C, and decent capacities delivered even at low temperature of −20 °C) highlights the potential of such quasi-solid-state lithium metal batteries as a viable solution for the next-generation high-performance lithium metal 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
CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Xi Wu,Xiaohua Jie,Xinghua Liang,Qicheng Hu,Liuyan Zhang,Jin Wang,Shufang Wu
Solid state lithium-ion batteries (SSLIBs) with high safety and high energy density are promising novel energy storage devices. However, the performance of SSLIBs would descend under a wide work temperature range. A flexible ceramic-polymer composite solid electrolyte membrane was created by solution casting to obtain good stability of SSLIBs at different temperatures. The PVDF-HFP-PES-LiClO 4 -Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) composite solid electrolyte shows excellent electrochemical performances in the temperature range of 20 to 60 o C. The ionic conductivity of PVDF-HFP-PES-LiClO 4 -LLZTO (PPLL) is 4.26 × 10 -4 , 4.97 × 10 -4 , 5.26 × 10 -4 , 5.59 × 10 -4 and 5.97 × 10 -4 S cm -1 at 20, 30, 40, 50 and 60 o C, respectively. The PPLL was employed in LiFePO 4 (LFP)/PPLL/Li batteries, and their properties were tested at 0.2 C. The test results show that the LFP/PPLL/Li battery has a good charge-discharge, rate, and cyclic performance at 20 - 60 o C. After 150 cycles with 0.2C at 30 o C and 60 o C, the capacity retention rates of 75.6% and 86.4%, respectively. This work provides an effective strategy for designing and preparing SSLIBs.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2019
·
IF 3.517
Linghong Xu,Guibin Li,Jianxin Guan,Lulu Wang,Jitao Chen,Junrong Zheng
Solid polymer electrolytes are promising candidates to replace the extensively used flammable liquid electrolytes in lithium batteries. However, pure polymer electrolytes seldom meet practical requirements because of their relatively low ionic conductivity and poor mechanical properties. Herein, we report a garnet (Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 , LLZTO)-doped composite polymer electrolyte (CPE) membrane for high performance lithium batteries. The CPE is composed of poly(vinylidene fluoride- co -hexafluoropropylene) (PVDF-HFP) and poly(ethylene glycol) methyl ether methacrylate (POEGMA) polymer with the addition of ceramic particles LLZTO. It not only has high ionic conductivity of 1.00 × 10 −3 S cm −1 after the activation of liquid electrolyte at room temperature, but also surprisingly restrains the growth of Li dendrites. Its electrochemical stability window is up to 4.7 V (vs. Li + /Li). Moreover, LiFePO 4 /Li batteries using the CPE exhibit excellent cycling performance and superior rate capability.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2023
·Vol. 36
·期 7
·2308275
·
IF 29.4
Xia Hu,Jiahao Yu,Yao Wang,Weiqian Guo,Xiang Zhang,Michel Armand,Feiyu Kang,Guoxiu Wang,Dong Zhou,Baohua Li
Lithium garnets are considered as promising solid-state electrolytes for next-generation solid-state Li metal batteries (SSLBs). However, the Li intrusion driven by external stack pressure triggers premature of Li metal batteries. Herein, for the first time, an in situ constructed interfacial shield is reported to efficiently inhibit the pressure-induced Li intrusion in SSLBs. Theoretical modeling and experimental investigations reveal that high-hardness metallic Mo nanocrystals inside the shield effectively suppress Li dendrite growth without alloy hardening-derived interfacial contact deterioration. Meanwhile the electrically insulated Li 2 S as a shield component considerably promotes interfacial wettability and hinders Li dendrite penetration into the bulk of garnet electrolyte. Interfacial shield-protected Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO)-based cells exhibit significantly enhanced cyclability without short circuits under conventional pressures of ≈0.2 MPa and even at high pressure of up to 70 MPa; which is the highest endurable stack pressure reported for SSLBs using garnet electrolytes. These key findings are expected to promote the wide-pressure-range applications of SSLBs.
研究领域:
材料科学
·
储能
·
电化学
·
固态电池
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）