Batteries-Basel
·
2023
·Vol. 9
·期 5
·257
·
IF 4
Xinjie Yu,Pengbo Zhai,Ning Zhao,Xiangxin Guo
Solid polymer electrolytes (SPEs) are seen as the key component in the development of solid-state lithium batteries (SSLBs) by virtue of their good processability and flexibility. However, poor mechanical strength, low room-temperature lithium-ion (Li-ion) conductivity and unsatisfactory interfacial compatibility with electrodes limit their practical application. In this work, a composite electrolyte consisting of polyvinylidene fluoride and polyvinylidene carbonate with a Li6.4La3Zr1.4Ta0.6O12(LLZTO) active filler (PFPC: LLZTO-SPE) is reported to achieve excellent ionic conductivity (4.25 × 10−4S cm−1at 30 °C), a wide electrochemical window (>4.6 V), a high Li-ion transference number (tLi+= 0.49) and good interfacial compatibility with the electrode. Incorporating LLZTO as an active filler not only increases the ionic conductivity of the electrolyte, but also homogenizes Li-ion flux and stabilizes the electrode/electrolyte interface, thereby preventing lithium dendrites from piercing the electrolyte. As a result, Li/Li symmetrical cells using PFPC: LLZTO-SPEs deliver more than 800 h of cyclability at 0.1 mA cm−2and a high critical current density (CCD) of 2.6 mA cm−2. The assembled Li/PFPC: LLZTO/LFP SSLBs achieve 87% capacity retention after 150 cycles at 0.2 C and 89% capacity retention for 100 cycles at 0.5 C. This work inspires new insights into designing high-performance SPEs.Keywords:LLZTO;in-situ polymerization;solid polymer electrolytes;solid-state 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
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Chaowei He,Hangjun Ying,Lucheng Cai,Hengquan Chen,Zuojie Xu,Shenwen Liu,Pengfei Huang,Haiyuan Zhang,Wenlong Song,Jian Zhang,Lu Shi,Weiwei Gao,Dan Li,Wei-Qiang Han
Solid-state lithium metal batteries (SSLMBs) with poly (ethylene oxide) (PEO)-based electrolytes have increasingly become one of the most promising battery technologies due to high energy density and safety. However, adverse electrode/electrolyte interface compatibility issues hinder further application. Herein, a PEO-based composite solid electrolyte with excellent anode and cathode interfacial compatibility is designed via the coordination modulation strategy induced by lithium difluorobis(oxalato)phosphate (DFBOP). By utilizing this electrolyte, the robust inorganic-rich interphase involving LiF, Li x PO y F z , and P─O components is in situ generated on lithium (Li) anode and LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode surfaces via forceful coordination among PEO, lithium bis(trifluoromethanesulphonyl)imide, and DFBOP and subsequent adjustment of front orbital energy levels. It contributes to homogeneous lithium deposition and an effective impediment of PEO oxidation decomposition at high voltage, promoting superior interfacial stability. Consequently, Li-symmetric cells with modified electrolyte can achieve a stable cycle over 7000 h at 0.2 mA cm −2 . Specially, the cathode electrolyte interphase with a unique organic–inorganic interpenetration network structure enables the 4.5 V Li/NCM811 cells to cycle steadily over 100 cycles, with a high discharge capacity of 215.4 mAh g −1 and initial coulombic efficiency of 91.23%. This research has shed light on the interfacial design of PEO-based electrolytes from the perspective of electrolyte coordination regulation to construct high-performance SSLMBs.
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 POWER SOURCES
·
2024
·
IF 8.1
Yuchen Wu,Ming Chao,Chengyi Lu,Hanyu Xu,Kai Zeng,Decheng Li,Ruizhi Yang
Surface functionalization is one effective strategy for optimizing the stability of Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) with Li metal anodes and the compatibility between the components of an electrolyte for lithium battery. Herein, a bifunctional modification layer induced by the silane coupling agent (SCA) and ionic liquid (IL) are successfully introduced onto the surface of LATP particles (defined as [email protected] ) through chemical grafting and ion exchange strategies. Benefitting from the synergistic effect between the protection of modification layer and the effectively reduced interaction of PEO chain segments with Li + , the compatibility of LATP with the Li metal anode is improved, and the dispersion of LATP in PEO matrix is enhanced, a faster Li + transfer is thereby enabled. As a result, thus-prepared [email protected] composite polymer electrolyte (CPE) shows an excellent electrochemical property with high ionic conductivity (1.455 × 10 −3 S cm −1 at 60 °C), enhanced Li-ion transference number (0.40), wide electrochemical stability window (4.76 V vs. Li + /Li) and favorable Li metal compatibility (over 1200 h). Furthermore, separately assembled Li/ [email protected] CPE/LFP coin full cells and pouch cells verify the operational feasibility under extreme conditions. This work paves a new way to protect LATP and promote its practical application in all-solid-state lithium batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Shenghan Li,Jiatang Wang,Feng Ji,Mingyin Wang,Zhenyuan Hu,Shikang Huo,Shuai Zhang,Hansong Cheng,Yunfeng Zhang
The interfacial compatibility between inorganic powder and polymeric matrix is one of the most important key factors for the applications of polymer ceramic composite electrolytes (PCCEs). In the present study, a surface modification strategy has been proposed by using three different terminating groups of silane coupling agents in the modification of the interfacial compatibility between LLZO and PEO in PEO/LLZO composite electrolyte. Experiments and density functional theory (DFT) calculations have been performed in studying the effect of different silane coupling agents on interfacial properties . Especially, the interface compatibility is found to be improved when using amino-terminated silane coupling agent KH550, which is due to hydrogen bond interactions between amino groups and PEO. In addition, the mechanical strength and conductivity are significantly increased by increasing the interaction energy and by decreasing the crystallinity , and the values of 1.39 MPa and 0.22 mS cm −1 at 30 °C are then successfully achieved. As a result, the solid-state LiFePO 4 |PCCE|Li battery demonstrates a high discharge specific capacity of 157 mAh g −1 at 60 °C and 1C. And it has a cycle capacity decay rate of only 0.034 % for 380 cycles. These results pave the way for future developments of high-performance PCCEs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2024
·
IF 18.9
Jiayi Zheng,Xieyu Xu,Jie Zhao,Xia Ma,Hui Wang,Kai Xie,Yu Han,Shizhao Xiong,Yuxiao Lin,Chunman Zheng,Qingpeng Guo
Solid-solid interfaces in the composite nickel-rich layered oxide LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode for solid-state lithium-metal batteries face the thorny issues of macroscopic contact interface, significant side reaction, intergranular cracking and sluggish Li + /e − transfer. To avoid such problems, we designed a high ionic/electronic dual-conducting soft gel coating on NCM811 cathode particles through the high-temperature semi-cyclized polyacrylonitrile strategy, aiming to build an unobstructed channel for enhanced transport kinetics in solid composite cathode. Additionally, an inner electrochemically stable interface layer is constructed between the coating layer and cathode particles vialing in situ electrochemical conversion. Thus, the coating layers with specific properties can maintain structural integrity of NCM811 cathode via buffering the internal stress during lithiation/delithiation and endows the solid-state battery with low interfacial resistance, outstanding cycling stability and thermal safety stability. Notably, this facile and scalable surface engineering provides a novel solution for the application of high nickel cathode materials in solid-state batteries.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
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
✓ 已验证
DOI
高影响因子
Interdisciplinary Materials
·
2022
·Vol. 1
·期 3
·434-444
·
IF 0
Guoxu Wang,Yuhao Liang,Hong Liu,Chao Wang,Dabing Li,Li-Zhen Fan
All-solid-state Li metal batteries (ASSLMBs) have been considered the most promising candidates for next-generation energy storage devices owing to their high-energy density and safety. However, some obstacles such as thick solid electrolyte (SSEs) and unstable interface between the solid-state electrolytes (SSEs) and the electrodes have restricted the practical application of ASSLBs. Here, the scalable polyimide (PI) film reinforced asymmetric ultra-thin (~20 μm) composite solid electrolyte (AU-CSE) with a ceramic-rich layer and polymer-rich layer is fabricated by a both-side casting method and rolling process. The ceramic-rich layer not only acts as a “securer” to inhibit the lithium dendrite growth but also redistributes Li-ions uniform deposition, while the polymer-rich layer improves the compatibility with cathode materials. As a result, the obtained AU-CSE demonstrates an ionic conductivity of 1.44 × 10 −4 S cm −1 at 35°C. The PI-reinforced AU-CSE enables Li/Li symmetric cell stable cycling over 1200 h at 0.2 mA cm −2 and 0.2 mAh cm −2 . Li/LiNi 0.6 Co 0.2 Mn 0.2 O 2 and Li/LiFePO 4 ASSLMBs achieve superior performances at 35°C. This study provides a new way of solving the interface problems between SSEs and electrodes and developing high-energy-density ASSLMBs for practical applications.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
ADVANCED MATERIALS
·
2024
·
IF 27.4
Ziyu Song,Mengyu Tian,Jing Zhu,Jiayi Chen,Wenfang Feng,Liubin Ben,Hailong Yu,Xuejie Huang,Michel Armand,Zhibin Zhou,Heng Zhang
The extremely high chemical reactivity of lithium metal (Li°) electrodes and its enormous volume change during repetitive cycles cause continuous interfacial degradations in prevailing organic electrolytes, thus deteriorating the cycling performances of rechargeable lithium metal batteries (LMBs). Herein, departing from traditional wisdom on the design of electrolyte components, a super SEI-forming anion (SSA), as an efficient percussor for building stable interphases on Li° electrode, is proposed. Comprehensive investigations related to the unique anion chemistry of SSA reveal that the sulfonate and polyfluoroalkyl functionalities synergistically contribute to uniform spatial distributions of designer interfacial species, greatly improving the surface coverage property and conformal ability of the resulting interphases. Consequently, the incorporation of SSA leads to significant improvements in the cyclability of Li° electrode (exceeding 575 mAh cm −2 before failure) and the corresponding rechargeable Li°||LiFePO 4 cells [a five-time increase in lifespan as compared to the benchmark cell with the popular SEI-forming anion bis(fluorosulfonyl)imide (FSI)]. The present work offers a paradigm shift to tame the notorious interfacial issues via upgraded anion chemistry, which can promote the practical development of rechargeable LMBs and other kinds of metal batteries.
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 POWER SOURCES
·
2023
·
IF 9.2
Qi Liu,Lei Li,Gang Liu,Xi He,Yanhua Niu,Guangxian Li
Polyionic liquids (PILs) are considered promising candidates for next−generation solid polymer electrolytes (SPEs) because they combine the electrochemical stability of ionic liquids with the processability/flexibility of polymers. However, the practical application of PILs−based SPEs are limited by their unsatisfactory mechanical properties in parallel with their insufficient ionic conductivity . Here, a double crosslinked PIL-based SPE with an optimal balance of ionic conductivity and mechanical properties is constructed by ultraviolet (UV) initiated polymerization. Among, the ionic liquid 1−(4−vinylbenzyl)−3−butylimidazolium bis(trifluoromethanesulfonyl)imide ([VBBIM][TFSI]) as a monomer , poly(ethylene glycol) diacrylate (PEGDA) and polyhedral oligomeric sesquisiloxane (POSS) as a functional crosslinker . As expected, the synthesized PIL−based SPE (POSS-PIL-PEGDA−1, 1 wt% POSS) shows a high ionic conductivity of 1.8 × 10 −4 S cm −1 (at 30 °C), a satisfactory tensile strength of 0.64 MPa, an ultrahigh thermal degradation temperature around 320 °C and a wide electrochemical stability window about 5.0 V versus Li/Li + . As a concept proof, the POSS-PIL-PEGDA−1 SPE can effectively inhibit lithium dendrites growth, and the assembled Li||LiFePO 4 solid−state lithium metal battery achieves a high discharge capacity and a good cycling performance. This strategy is attractive for studying the trade−off between mechanical properties and ionic conductivity of crosslinked PIL−based SPEs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Batteries-Basel
·
2023
·Vol. 9
·期 6
·320
·
IF 4
Zhenghang Zhang,Rongzheng Fan,Saifang Huang,Jie Zhao,Yudong Zhang,Weiji Dai,Cuijiao Zhao,Xin Song,Peng Cao
Solid composite electrolytes exhibit tremendous potential for practical all-solid-state lithium metal batteries (ASSLMBs), whereas the interfacial contact between cathode and electrolyte remains a long-standing problem. Herein, we demonstrate an integrated design of a double-layer functional composite electrolyte and cathode (ID-FCC), which effectively improves interfacial contact and increases cycle stability. One composite electrolyte layer, PVDFLiFSI@LLZNTO (PL1@L), comes into contact with the LLZNTO (Li6.5La3Zr1.5Nb0.4Ta0.1O12)-containing cathode, while the other layer, PEOLiTFSI@LLZNTO (PL2@L) with a Li anode, is introduced in each. Such a design establishes a continuous network for the transport of Li+on the interface, and includes the advantages of both PEO and PVDF for improving stability with the electrodes. The Li symmetric cells Li/PL2@L-PL1@L-PL2@L/Li steadily cycled for more than 3800 h under the current density of 0.05 mA cm−2at 60 °C. Outstandingly, the all-solid-state batteries of LiFePO4-ID-FCC/Li showed an initial specific capacity of 161.5 mA h g−1at 60 °C, demonstrating a remaining capacity ratio of 56.1% after 1000 cycles at 0.1 C and 74.5% after 400 cycles at 0.5 C, respectively. This work provides an effective strategy for solid-state electrolyte and interface design towards ASSLMBs with high electrochemical performance.Keywords:all-solid-state lithium batteries;inorganic-polymer hybrid electrolyte;double-layer integrated design;garnet oxide (LLZNTO);cycle stability
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS ENGINEERING AND PERFORMANCE
·
2021
·Vol. 30
·期 6
·4543-4551
·
IF 1.819
Liu Fangfang,Chuan Xiuyun,Yang Yang,Huang Dubin,He Xin
Solid-state lithium batteries using solid-state electrolytes (SSE) improve both thermal stability and energy density compared with organic liquid electrolytes lithium-ion batteries (LIBs). However, their usage is still challenged by low lithium-ion conductivity and high interfacial resistance between SSE and electrodes, as well as difficulties running at room temperature (RT). Herein, we demonstrate an electrode/solid-state electrolyte interface, in which poly(ether-acrylate) (PEA) network was introduced on the surface of ceramic electrolytes via photo-polymerization, thus dramatically reducing the SSE/Li interfacial resistance from 4822 to 122 Ω cm 2 . As a result, the Li/Li cells can cycle over 500 h at 0.3 mA cm −2 , LiFePO 4 /Li delivers 200 cycles with capacity retention of 91.1% at RT, respectively. This research provides a method to improve the interface contact between SSE and electrodes, and offers possibilities for application of solid-state Li metal batteries under ambient condition.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2023
·
IF 6.4
Zhuangzhuang Xue,Yan Zhang,Zehua Zhao,Xiaowei Shi,Haitao Zhao,Keyu Cheng,Jiamei Liu,Lei Li
The practical application of poly(ethylene oxide) (PEO)-based electrolytes in all-solid-state lithium metal batteries is hindered by its low ionic conductivity at room temperature, resulting from the high crystallinity of PEO. Decreasing the crystallinity of PEO can increase the ionic conductivity of PEO-based electrolytes but sacrifice its mechanical property that also affects its practical application. Herein, we design and experimentally realize a completely amorphous PEO-based electrolyte with promising high mechanical strength. It is a glass fiber-reinforced PEO-based electrolyte functionalized with nano-LiF and succinonitrile additives. The electrolyte has 0 crystallinity and a high tensile strength of 6.06 MPa, resulting in a high ionic conductivity (2.6 × 10–4 S/cm, 25 °C) and a widened electrochemically stable window (4.9 V). It also has good interfacial stability with lithium and can stably work for 500 h in symmetrical lithium batteries (Li/Li) at 25 °C and 0.2 mA/cm2. It is also evaluated in all-solid-state batteries with LiFePO4 as the cathode and Li as the anode and shows promising electrochemical performance. This work provides a solution for the development of high-performance PEO-based solid-state batteries operating normally at room temperature.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）