SOLID STATE IONICS
·
2020
·
IF 3.107
Xuefeng Shen,Qian Zhang,Tianxiang Ning,Jianlei Liu,Taoyong Liu,Zhiwei Luo,Yao He,Chunchun Qin,Anxian Lu
Garnet solid electrolyte is the most promising candidate among inorganic solid electrolytes due to its wide potential window, good compatibility and high safety. In this work, a dual doping strategy is offered for the development of garnet-type electrolytes with high ionic conductivity . Te 6+ is introduced into the Zr sites to stabilize the high-ionic conductivity cubic phase. Simultaneously, Sr 2+ enter the La sites to achieve a fine-tuning of the Li + concentration by charge compensation, acting as a sintering agent of Te 6+ /Sr 2+ doped electrolytes. The structure, chemical composition and ionic conductivity of Li 7 − 2 y + x La 3 − x Sr x Zr 2 − y Te y O 12 ( x = 0–0.25, and y = 0.35) electrolytes are systematically investigated by X-ray diffraction, Raman spectroscopy , scanning electron microscope , Energy Dispersive X-ray Spectroscopy, Inductively Coupled Plasma-Optical Emission Spectrometry and Alternating Current impedance. The results show that the optimal amount of Sr 2+ substitution helps to reduce the total resistance by promoting the growth of grains and ceramic densification . Among the investigated compositions, the composition with Li 6.425 La 2.875 Sr 0.125 Zr 1.65 Te 0.35 O 12 exhibits excellent performance with relative density of 97.95%, conductivity of 4.27 × 10 −4 S cm −1 at 25 °C and activation energy of 0.30 eV. The assembled Li/Li 6.425 La 2.875 Sr 0.125 Zr 1.65 Te 0.35 O 12 /Li symmetrical batteries are cycled galvanostatically under different current densities. The results show that the symmetrical battery can achieve good cyclic stability, good Li + stripping and plating process and low overpotential.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Cheng Ouyang,Hongpeng Zheng,Qiwen Chen,Hezhou Liu,Huanan Duan
Solid-state lithium batteries hold great promise for next-generation energy storage systems. However, the formation of lithium filaments within the solid electrolyte remains a critical challenge. In this study, we investigate the crucial role of morphology in determining the resistance of garnet-type electrolytes to lithium filaments. By proposing a new test method, namely, cyclic linear sweep voltammetry, we can effectively evaluate the electrolyte resistance against lithium filaments. Our findings reveal a strong correlation between the microscopic morphology of the solid electrolyte and its resistance to lithium filaments. Samples with reduced pores and multiple grain boundaries demonstrate remarkable performance, achieving a critical current density of up to 3.2 mA cm–2 and excellent long-term cycling stability. Kelvin probe force microscopy and finite element method simulation results shed light on the impact of grain boundaries and electrolyte pores on lithium-ion transport and filament propagation. To inhibit lithium penetration, minimizing pores and achieving a uniform morphology with small grains and plenty of grain boundaries are essential.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
·
2022
·Vol. 37
·期 2
·149-154
·
IF 1.271
Sun Jiyang,Li Yiqiu,Guo Xiangxin
Li/garnet/LiFePO 4 solid-state battery was fabricated. The cathode contains LiFePO 4 , Ketjen black, poly(vinylidene fluoride):LiTFSI polymer as active material, electric conductor and Li-ion conducting binder, respectively. Polyvinylpyrrolidone was added into the cathode to improve cathode/electrolyte interfacial performance. When combined with polyvinylpyrrolidone additive, poly(vinylidene fluoride):polyvinylpyrrol idone:LiTFSI blend forms, and the cathode/electrolyte interfacial resistance reduces from 10.7 kΩ to 3.2 kΩ. The Li/garnet/LiFePO 4 solid-state battery shows 80% capacity retention after 100 cycles at 30 °C and 0.05 C. This study offers a general strategy to improve cathode/electrolyte interfacial performance and may enable the practical application of solid-state Li-metal 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
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Li Yang,Xiao Huang,Changfei Zou,Xiyuan Tao,Lei Liu,Kaili Luo,Peng Zeng,Qiushi Dai,Yongfang Li,Lingguang Yi,Zhigao Luo,Xianyou Wang
Lithium-sulfur (Li–S) batteries are attractive due to their high theoretical energy density . However, conventional Li–S batteries with liquid electrolytes undergo polysulfide shuttle-effect and lithium dendrite formation during charge/discharge process, leading to poor electrochemical performance and safety issues. Garnet type Li 7 La 3 Zr 2 O 12 (LLZO) solid-state electrolyte (SSE) restricts the penetration of polysulfides and exhibits high ionic conductivity at room temperature (RT). Herein, Li 6.5 La 3 Zr 1.5 Nb 0.5 O 12 (LLZNO) ceramic electrolyte using Li 3 PO 4 (LPO) as sintering aids (LLZNO-LPO) is prepared by the rapid sintering method and is applied to construct a shuttle-effect free solid-state Li–S battery . The SSE displays high conductive pure cubic-LLZO phase; during the rapid sintering, LPO melts and junctions the voids between the grains, thus improves Li + conductivity. As a result, the LLZNO-LPO ceramic electrolyte with Li + conductivity of 4.3 × 10 −4 S cm −1 and high critical current density (CCD) of 1.2 mA cm −2 is obtained at RT. The Li–S solid-state battery which utilizes LLZNO-LPO ceramic electrolyte can deliver an initial discharge capacity of 943 mA h·g −1 and 602 mA h·g −1 retention after 60 cycles. In the same time, the initial coulombic efficiency is as high as 99.5%, indicating that the SSE can effectively block the polysulfide shuttle towards the Li anode and fulfill a shuttle-free Li–S battery.
研究领域:
材料科学
·
电化学
·
能源存储
·
固体离子学
·
先进电池技术
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Xianzhun Huang,Haojie Liu,Wenyi Xiang,Lihan Chen,Xinran Li,Bangzhuang Xue,Jian Ma,Yueyue Wu,Chengwei Wang,Yinhua Bao,Weiwei Ping
Oxide-based electrolytes are promising with high ion conductivity and a wide electrochemical window (0–5 V). However, the brittleness and poor compressibility severely inhibit their application. Here, inspired by the “flexible eggshell membrane”, we fabricated a 20 µm, flexible and compressible Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 thin film by in-situ healing the LLZTO crystal chips with poly(di(ethylene glycol) ethyl ether acrylate) electrolytes. Fracture mechanics analysis demonstrates the superior mechanical properties of the flexible LLZTO films. With the package pressure increasing from 0.6 to 1.4 t, the Li metal symmetric cell displays a decreasing internal resistance from ∼281 to ∼156 Ω cm 2 , corresponding to the low limit of ion conductivity from ∼0.6 × 10 −4 to ∼2.1 × 10 −4 S/cm. The symmetric cell can be a stable cycle for ∼220 h at 0.4 mA/cm 2 and ∼300 h at 0.1 mA/cm 2 with a bending angle of 30°. The full cell LiFePO 4 /LLZTO/Li shows a superior rate performance of 150 mA/g and a long cycle life of ∼200 cycles. Pairing with the LiNi 0.8 Co 0.1 Mn 0.1 O 2 , the cell displays a Coulombic efficiency of ∼99.7 % for ∼150 cycles. These results indicate that we have successfully fabricated flexible and compressible LLZTO films, and this will open an avenue for the application of high-energy-density thin film batteries.
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 35
·期 8
·2415542
·
IF 18.5
Meiqi Jia,Ting-Ting Wu,Si-Dong Zhang,Sijie Guo,Yongzhu Fu,An-Min Cao
Garnet-type solid-state electrolytes (SSEs) exemplified by Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZT) are chemically unstable when exposed to air, leading to the formation of impurities and poor wettability with Li metal. Herein, a protocol to address this Li/LLZT interface challenge is demonstrated by constructing a lithiophilic MgF 2 nanofilm on the LLZT pellet. Specifically, a solution-based process is developed for the surface engineering of LLZT, utilizing magnesium trifluoroacetate (MTF) as the molecular precursor while poly(acrylic acid) (PAA) as the coordinating agent in a sol-gel process. It is demonstrated that a facile spin-coating treatment followed by high-temperature annealing reliably forms crack-free MgF 2 nanofilms with precise thickness control. Introduction an MgF 2 interlayer transforms the LLZT pellet into a highly lithophilic, facilitating close contact with the lithium anode, thereby leading to a significantly reduced interfacial resistance from 1190 Ω cm 2 to 6 Ω cm 2 . Such an interfacial engineering enables stable cycling of full batteries with high reversibility and rate capability using commercial LiFePO 4 and LiNi 0.83 Co 0.07 Mn 0.1 O 2 as cathodes. This study unfolds the possibility of a solution-based method as a facile and scalable process for the construction of fluoride nanofilms, which is promising to address the critical interfacial challenges of solid-state batteries (SSBs) to facilitate its practical applications.
研究领域:
材料科学
·
储能
·
电化学
·
固体离子学
·
纳米薄膜制备
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Yidong Jiang,Jun Ma,Anjie Lai,Wei Huang,Chaoyang Wang,Shang-Sen Chi,Jun Wang,Yonghong Deng
Garnet-based all-solid-state lithium batteries are expected to achieve high energy density and safety. However, the distinctly different chemical and electrochemical environment between the electrodes and garnet-type Li 6·4 La 3 Zr 1·6 Ta 0·4 O 12 (LLZTO) electrolyte results in high interfacial impedance that greatly hinders the electrochemical performance . Herein, we propose an asymmetrical interface modification strategy by respectively introducing an ultrathin in-situ polymerized interlayer on the cathode side and a lithiophilic liquid metal coating layer on the Li metal anode side. As a result, the interfacial impedance on both side is significantly reduced to 214 Ω cm 2 on the cathode side and 7.45 Ω cm 2 on the Li metal anode side due to the intimate contact and enhanced wettability between Li metal and GSSE together with improved conformability on the cathode side and Li ion conductance within the cathode. Therefore, the interface modified LiFePO 4 ||LLZTO||Li all-solid-state battery exhibits excellent cycling performance over 150 cycles with capacity retention of 96.7% and small voltage polarization of 55 mV at 0.1C and 60 °C. This work provides a convenient strategy to alleviate the interfacial issues in all-solid-state batteries.
研究领域:
电化学
·
材料科学
·
能源存储
·
固态离子学
·
电池技术
·
界面工程
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhang Nian,Ren Guoxi,Li Lili,Wang Zhi,Yu Pengfei,Li Xiaobao,Zhou Jing,Zhang Hui,Zhang Linjuan,Liu Zhi,Liu Xiaosong
Garnet-type Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZO) is considered a promising solid electrolyte, but the surface degradation in air hinders its application for all-solid-state battery. Recent studies have mainly focused on the final products of the LLZO surface reactions due to lacking of powerful in situ characterization methods. Here, we use ambient pressure X-ray spectroscopies to in situ investigate the dynamical evolution of LLZO surface in different gas environments. The newly developed ambient pressure mapping of resonant Auger spectroscopy clearly distinguishes the lithium containing species, including LiOH, Li 2 O, Li 2 CO 3 and lattice oxygen. The reaction of CO 2 with LLZO to form Li 2 CO 3 is found to be a thermodynamically favored self-limiting reaction. On the contrary, the reaction of H 2 O with LLZO lags behind that of CO 2 , but intensifies at high pressure. More interestingly, the results provide direct spectroscopic evidence for the existence of Li + /H + exchange and reveal the importance of the initial layer formed on clean electrolyte surface in determining their air stability. This work demonstrates that the newly developed in situ technologies pave a new way to investigate the oxygen evolution and surface degradation mechanism in energy materials.
研究领域:
材料科学
·
电化学
·
固态电池
·
表面化学
·
光谱学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）