ENERGY & FUELS
·
2026
·Vol. 40
·期 35
·19765-19777
·
IF 6
Yang Zhitao,Liu Yulei,Fu Xiuwen,Xu Weiheng,Liu Jinpeng
Poly(ethylene oxide) (PEO)-based solid polymer electrolytes
are
promising for solid-state lithium metal batteries because of their
favorable flexibility, processability, and lithium-salt solvation
capability. However, their practical application is still limited
by insufficient ion transport, a low lithium-ion transference number,
and poor lithium-metal interfacial stability. Herein, dual-lithium-salt-regulated
composite polymer electrolytes (DSCPEs) were constructed by incorporating
a LiTFSI/LiDFOB dual-salt system into a PEO–LLZTO composite
polymer electrolyte matrix to achieve a balance between ion transport
capability and lithium-metal interfacial stability. The optimized
DSCPE-2 (LiTFSI:LiDFOB = 3:2) delivers an ionic conductivity of 6.63
× 10 –4 S cm –1 , a lithium-ion
transference number of 0.69, and an electrochemical stability window
of up to 5.1 V. In addition, the Li|DSCPE-2|Li symmetric cell operates
stably for over 2000 h at 60 ° C under 0.1 mA cm –2 , with a critical current density of 1.05 mA cm –2 , indicating its enhanced compatibility with lithium metal. When
assembled with a LiFePO 4 cathode, the Li|DSCPE-2|LFP full
cell delivers an initial discharge capacity of 136.54 mAh g –1 and retains 123.41 mAh g –1 after 300 cycles at
0.5 C and 60 ° C, corresponding to a capacity retention of 90.38%.
Furthermore, the cell maintains a reversible capacity of approximately
115 mAh g –1 even at 5 C. This work provides an effective
strategy for regulating ion transport behavior and lithium–metal
interfacial stability in PEO-based composite polymer electrolytes.
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Shidong Song,Yongqiang Xu,Yanli Ruan,Hong Wang,Dequan Zhang,Joykumar Thokchom,Donghai Mei
Amorphous Li–La–Zr–O (LLZO) solid-state electrolyte thin films are promising alternatives to the well-established lithium phosphorus oxynitride (LiPON) electrolyte for all-solid-state lithium batteries due to their potentially higher Li-ion conductivity and stability. Herein, the enhancement methodology in the ionic conductivity of amorphous LLZO-based thin films is investigated. By doping with Ta, the conductivity of the amorphous LLZO film at 30 °C (3.9 × 10–7 S cm–1) can be enhanced by up to an order of magnitude (2.6 × 10–6 S cm–1), ascribed to tuning Li conduction in local near-order LLZO nanodomains. On that basis, an isomeric Li–La–Zr–Ta–O (LLZTO) amorphous–crystalline composite thin film is prepared via incorporating cubic LLZTO particles into the amorphous LLZTO matrix. The composite film with 10 wt % cubic LLZTO filler can further achieve an ionic conductivity of 0.8 × 10–5 S cm–1 at 30 °C, which is comparable to the best values obtained for the state-of-art LLZO-based thin films. Li transport through the well-connected cubic LLZTO filler network and along the interfaces between the crystallites and the amorphous matrix in the LLZTO composite thin film may offer fast and long-range Li-conduction pathways, which supplement the ionic conduction in the amorphous matrix with short-range-ordered and long-range-disordered structures.
研究领域:
材料科学
·
能源存储
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DOI
高影响因子
Materials Today Energy
·
2024
·
IF 9
Jiechen Song,Yuxing Xu,Yuncheng Zhou,Rui He,Aijia Wei,Qiangqiang Tan
Lithium metal batteries with polyethylene oxide (PEO) electrolytes have shown great potential to be one of the next-generation energy candidates. As the branch family of PEO electrolytes, poly(ethylene glycol) acrylates (PEGAs) attract more attention owing to their better electrochemical properties than that of PEO electrolytes. Introducing double bond-modified Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 fillers (KH@LLZTO) has been a popular method to improve the electrochemical properties of PEGAs electrolytes due to the homogeneous dispersion of LLZTO. However, in this work, an inverse phenomenon is discovered. The electrochemical properties of PEGAs electrolytes get worse when introducing KH@LLZTO. By exploring the Li + transport mechanism, the reason for the inverse phenomenon is revealed. More importantly, the design principle of PEGAs electrolytes with fast ionic conductor fillers is presented. Double bond-modified LLZTO can decrease the electrochemical properties of PEGAs electrolytes instead when there are low-molecular weight monomers that can participate in the PEGAs polymer network and interact with Li + , while the double bond-modified LLZTO can improve the electrochemical properties of PEGAs electrolytes when there are not aforementioned low-molecular weight monomers. This work provides a new understanding for componential design and optimization of PEGAs electrolytes with fast ionic conductors, hoping to promote the practical application of PEGAs electrolytes.
研究领域:
材料科学
·
电化学
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高影响因子
Batteries & Supercaps
·
2023
·Vol. 6
·期 6
·e202300056
·
IF 5.7
Yuxiang Liu,Furui Ma,Wenpeng Li,Ligang Gai,Haohua Yang,Zengqi Zhang
Graphical A solid polymer electrolytes (SPEs) with polymerized ionic liquid and LLZTO was prepared by common solution casting method. Solid-state batteries assembled with it displayed excellent charge-discharge performance and cycling stability. Solid polymer electrolytes (SPEs) combine the benefits of ceramic electrolyte and polymer electrolyte, and have broad application prospects in high-energy lithium metal batteries. However, low Li + conductivity and tensile strength are crucial elements that hinder the application of solid polymer electrolytes. In this paper, an effective solid polymer electrolyte was proposed to solve these problems. A polymerized ionic liquid (PIL) was chosen as the ionic transport material to synthesize three-dimensional cross-linked ion channels through thermal polymerization, which can effectively improve the ionic conductivity. This work is different from some other reports that add ionic liquid without C=C double bond. We used the vinyl ionic liquid (IL) as matrix via polymerization with azobis initiator (AIBN) and the obtained co-polymer has excellent flexibility and non-flowing character. Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) ceramic filler was added to enhance the thermal stability and tensile strength of the electrolyte. Meanwhile, solid-state batteries (SSBs) assembled with LiFePO 4 cathode and high-voltage LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode can deliver remarkable cell performance. This work presents an appropriate device for the structure of modern polymerized ionic liquid solid polymer electrolytes, and shows significant implication for the progress of high-property polymer electrolytes.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Lei Liu,Kaiqi Wu,Liyuan Huang,Liang Lan,Dong Cheng,Hanyu Yi,Xin Ao,Yecheng Liu,Chengjin Peng,Shan Fang
Composite polymer electrolytes (CPEs) used in solid-state lithium metal batteries (SSLBs) continue to face challenges, including a gradual rise in interfacial resistance and unchecked growth of lithium dendrites. Herein, a flexible and mechanically robust sandwich-structured CSE membrane is constructed, features poly(vinylidenefluoride-co-trifluoroethylene) (P(VDF-TrFE)) containing 4 wt% Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) used on the top and bottom, with a central layer compose of 70 wt% LLZTO with P(VDF-TrFE), refers to PTL4. The flexible outer layers enriched in polymer, provide excellent electrode contact, while the rigid middle layer characterized by a high content of LLZTO, effectively impedes lithium dendrite penetration and enhances Li + conductivity. The as prepared PTL4 exhibits high ionic conductivity of 1.02 × 10 −4 S cm −1 at 30 °C, a wide electrochemical window up to 4.9 V, and outstanding mechanical properties (tensile strength of 8.9 MPa and 150 % strain). The symmetric Li|PTL4|Li cells demonstrate stable cycling performance for over 1500 h at 30 °C. Moreover, Li|PTL4|LiFePO 4 cells maintain exceptional capacity of 98 % after 250 cycles at a high rate of 0.5C, accompanied by an average Coulombic efficiency exceeding 99.5 %. Furthermore, the fabricated pouch cells are characterized by their foldability, cutability, and puncture resistance, underscoring their potential to enhance battery safety.
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高影响因子
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
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Dingsheng Shao,Li Yang,Kaili Luo,Manfang Chen,Peng Zeng,Hong Liu,Lei Liu,Baobao Chang,Zhigao Luo,Xianyou Wang
Lithium-sulfur (Li-S) batteries have become candidate for the next-generation energy storage systems because of their high energy density and specific capacity. However, due to the shuttle effect of polysulfides and the safety problems caused by liquid organic electrolytes, practical commercial applications of Li-S battery have been severely limited. With the recent development of solid electrolyte, the strategy of replacing liquid electrolyte with the solid electrolyte has aroused extensive attention, which can both improve the safety of the battery and increase its energy density. However, in the absence of liquid components, poor interfacial contact and low ionic conductivity for solid electrolyte can seriously impair the electrochemical performance of solid-state Li-S batteries. By adding a certain amount of liquid plasticizer, the ionic conductivity is effectively ameliorated and the interface contact between the electrodes and the electrolyte is largely improved. Herein, a thermally polymerized composite gel polymer electrolyte (CPE) for quasi-solid-state Li-S battery is designed and fabricated. The CPE has a satisfactory ionic conductivity and wide electrochemical window of above 4.5 V. Especially, the addition of the garnet Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 (LLZTO) powder improves the flame retardancy and thermal stability. In addition, the application of CPE in the Li-S battery can block the shuttle of polysulfide to some extent, and the quasi-solid-state Li-S battery assembled by CPE shows the good electrochemical performance and only a 0.22% decay per cycle in 200 cycles with 0.1C. Hence, this work provides a new strategy for design and development of the quasi-solid-state electrolyte for the application of Li-S battery. Moreover, due to its wide electrochemical window, CPE can also be applied in high-voltage cathode systems of lithium ion battery in the future.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 36
·20633-20639
·
IF 10.733
Huilin Xie,Chunli Li,Wang Hay Kan,Maxim Avdeev,Chenyou Zhu,Zhikun Zhao,Xiaorong Chu,Daobin Mu,Feng Wu
All solid-state batteries have received significant attention due to their excellent safety performance. As a key component, the garnet-type electrolyte is one of the best known electrolytes due to its air stability and good compatibility with metallic lithium. However, the total Li+ conductivity of this kind of electrolyte is usually lower than that of the bulk electrolyte primarily due to the grain boundary resistance. In this study, we focused on engineering the electrolyte Li6.4La3Zr1.4Ta0.6O12 (LLZTO) by introducing Li3BO3 (LBO) into it to form the electrolyte LLZTO/LBO with the aim to consolidate the grain boundary. Via characterization by both neutron and X-ray diffraction, the as-prepared LLZTO was indexed as a pure cubic phase, where Ta certainly substituted the Zr sites. LLZTO/LBO still maintained the cubic structure, and the B atoms did not occupy any cation sites in the unit cell. It was demonstrated that an amorphous phase of a boracic substance was trapped inside the cubic LLZTO phase. The amorphous boracic phase sutured the gaps among the LLZTO grains and then lowered the grain boundary resistance without introducing impurities, ultimately consolidating the solid-state electrolyte. Electrochemical impedance spectroscopy revealed that the total Li+ conductivity of LLZTO/LBO reached 5.47 × 10−4 S cm−1, much higher than those of the as-prepared Li7La3Zr2O12 (LLZO) and LLZTO. Using LLZTO/LBO as an electrolyte, the LiNi0.8Co0.1Mn0.1O2/LiFePO4 hybrid solid battery showed an excellent cycling performance with the reversible capacity of 147.8 mA h g−1 at 0.2C for 100 cycles and the capacity retention of 93.8%. These results suggest that the consolidation of the grain boundary with LBO is a promising way to achieve an improved electrolyte, LLZO, with higher total Li+ conductivity.
研究领域:
材料科学
·
电化学
·
储能技术
·
固态电池
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DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Tao Jiang,Bowen Zhu,Haiyun Shen,Ying Liu,Hao Liu,Wei Zheng,Mengtao Wu,Ning Xu,Li Chen
The Ni-rich LiNixCoyMn1–x–yO2 with high specific capacity and superior thermal stability under a high cutoff voltage (>4.3 V) will play a critical role in high-power lithium-ion batteries (LIBs). In this paper, LiNi0.8Co0.1Mn0.1O2 (NCM811) equipped with a stable garnet ceramic Li6.5La3Zr1.5Ta0.5O12 (LLZTO) nanoshell is successfully synthesized via a simple wet chemical approach. X-ray diffraction, scanning electron microscope (SEM), energy-dispersive spectrometer (EDS) element mapping, and transmission electron microscopy (TEM) confirm the presence of LLZTO on the NCM811 surface. The NCM811 with 2 wt % LLZTO (2-NCM811) can deliver a superior specific capacity of 144.4 mAh·g–1 at 1C (2.8–4.3 V) after 100 cycles, accompanied by a capacity retention rate as high as 81.1%. But pristine NCM811 has a discharge capacity of only 119.6 mAh·g–1 and a capacity retention rate as low as 69.5% under the same condition. What is more, 2-NCM811 exhibits an enhanced discharge capacity of 129.6 mAh·g–1 at 1C (2.8–4.5 V) after 100 cycles and a high capacity retention rate of 62.9%, which are superior to those of pristine NCM811 (110.0 mAh·g–1, 57.6%). The improved high-potential performance of 2-NCM811 can be attributed to the positive role of the LLZTO shell, which enhances the structural stability and simultaneously inhibits adverse side reactions at the surface of 2-NCM811 during cycling. Based on the above advantages, LLZTO with three-dimensional (3D) diffusion pathways and high ion conductivity is expected to be the most prospective material for the surface modification engineering of nickel-rich cathode materials in lithium-ion batteries (LIBs).
研究领域:
材料科学
·
电化学
·
储能技术
·
锂离子电池
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DOI
高影响因子
Batteries-Basel
·
2023
·Vol. 9
·期 10
·490
·
IF 4
Kang-Feng Chang,Pradeep Kumar Panda,Chien-Te Hsieh,Po-Chih Yang,Navish Kataria,Kuan Shiong Khoo
In this study, robust composite solid electrolytes were developed and employed to enhance the performance of Li-metal batteries significantly. The robust composite solid electrolytes are composed of a soft polymer, poly(ethylene oxide), a Li salt, bis(trifluoromethanesulfonyl)imide (LiTFSI), and super ionic conductive ceramic fillers such as Li1.5Al0.5Ti1.5(PO4)3(LATP), and Li6.4La3Zr1.4Ta0.6O12(LLZTO). The main goal of this study is to enhance the electrochemical stability and ionic conductivity. The ionic conductivities of the composite solid electrolytes were found to be 2.08 × 10−4and 1.64 × 10−4S cm−1with the introduction of LATP and LLZTO fillers, respectively. The results prove that the fabricated solid electrolyte was electrochemical stable at voltage exceeding 4.25 V vs. Li/Li+. The internal resistance of the solid electrolyte significantly reduced compared to gel electrolyte. This reduction can be attributed to the alleviation of bulk electrolyte, charge-transfer, and interfacial electrolyte/electrode impedance. When LiFePO4cathode sheets are coated with a composite solid electrolyte containing LATP powders, the resulting Li-metal battery displays high capacity at 5 C (with a capacity retention of 65.2% compared to the original capacity at 0.2 C) as well as superior cyclic stability and excellent Coulombic efficiency (>99.5%, 200 cycles). These results confirm that the composite solid electrolyte acts as a protective layer which has the ability to prevent the growth of Li dendrites. Consequently, the fabricated electrolyte configuration can be engineered to enable high energy/power density and electrochemical stable cyclability in Li-metal batteries.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Rong-Ao Tong,Linhui Chen,Gang Shao,Hailong Wang,Chang-An Wang
With the increasing demand for higher energy density Lithium-ion batteries, the battery safety issue has gained growing attention. Solid-state electrolytes (SSEs) are considered a promising solution to the volatilization and inflammable problems of the traditional liquid electrolytes . In this work, we propose a novel solvent-free modification process using stearic acid as a modifying agent for LLZTO/PEO hybrid electrolytes. Compared to the conventional solvent-casting process, the new one integrates surface modification and composite in a successive solvent-free step, so it can greatly improve the process efficiency and meet the requirement of green chemistry. Fourier Transform Infrared spectrometry (FTIR), X-Ray Diffraction (XRD) and Transmission Electron Microscope (TEM) observation confirm the structure of the uniform coating layer . The solvent-free modification and composite process are proved to significantly inhibit the agglomeration of LLZTO particles and the side reactions on particle surfaces in the polymer matrix by using Scanning Electron Microscope (SEM) and Thermal Gravimetric-Differential Thermal Analysis (TG-DTA) characterization. Thus, the prepared electrolyte has the ionic conductivity of up to 8.3 × 10 −4 S cm −1 at 70 °C. It has better electrochemical stability as well, which can achieve about 900 cycles in Li symmetric cells with a current density of 0.1 mA cm −2 .
研究领域:
材料科学
·
能源技术
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 11
·110537
·
IF 4.316
Fei Chen,Leana Ziwen Rannalter,Xing Xiang,Yanhua Zhang,Shangbin Song,Shiyu Cao,Qiang Shen
The development of solid electrolytes is a key step to break through the technical bottleneck of lithium batteries and obtain lithium batteries with high safety and high energy density. Combining the advantages of both inorganic and organic solid electrolytes, the form of inorganic fillers for composite solid electrolytes is extended from nanoparticles, nanofibers to a 3D matrix. In this study, a porous Li6.4La3Zr1.4Ta0.6O12 (LLZTO) ceramic framework was fabricated by adding a pore-forming agent, which was then infiltrated by succinonitrile (SN)-LiTFSI to take full advantage of the inorganic and organic parts of the composite electrolyte. The interconnected porous structure allows continuous ion transport pathways in both parts. The effect of the porosity, namely the amount proportion of inorganic and organic materials, on the electrochemical performance of composite electrolytes was investigated by regulating the amount of pore-forming agent. The presented composite solid electrolyte achieves a very high ionic conductivity of 1.08 × 10−3 S cm−1 at 30 °C, while it is stable up to 5.1 V at room temperature. The repeated lithium stripping/plating is stable over 250 h without short circuit.
研究领域:
材料科学
·
电化学
·
能源存储
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）