JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yali Liu,Youlong Xu,Yuan Zhang,Cheng Yu,Xuekai Sun
Composite solid electrolytes (CSEs) exhibit great potential due to their advantages of both sufficient strength and high ionic conductivity . However, their interfacial impendence and thickness hinder potential applications. Herein, a thin CSE with good interface performance is designed through the combination of immersion precipitation and in situ polymerization. By employing a nonsolvent in immersion precipitation, a porous poly(vinylidene fluoride-cohexafluoropropylene) (PVDF-HFP) membrane could be rapidly created. The pores in the membrane could accommodate sufficient well-dispersed inorganic Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) particles. Subsequent in situ polymerized 1,3‑dioxolane (PDOL) further protects LATP from reacting with lithium metal and supplies superior interfacial performance. The CSE has a thickness of ∼ 60 μm, ionic conductivity of 1.57 × 10 −4 S cm −1 , and oxidation stability of 5.3 V. The Li/1.25LATP-CSE/Li symmetric cell has a long cycling performance of 780 h at 0.3 mA cm −2 for 0.3 mAh cm −2 . The Li/1.25LATP-CSE/LiFePO 4 cell exhibits a discharge capacity of 144.6 mAh/g at 1C and a capacity retention of 97.72 % after 300 cycles. Continuous depletion of lithium salts due to the reconstruction of the solid electrolyte interface (SEI) may be responsible for battery failure. The combination of the fabrication method and failure mechanism gives new insight into designing CSEs.
研究领域:
材料科学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Lingguang Yi,Xiaoyi Chen,Jiajia Huang,Jiali Liu,Honghui Hu,Huahui Zhao,Tianjing Wu,Li Liu,Xianyou Wang
The sodium superionic conductor structure (NASICON) Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) is a promising active filler for its high ionic conductivity and air stability. Nonetheless, its large-scale application remains limited by chemical instability with lithium anodes. Herein, a novel poly(vinylidene fluoride- co -hexafluoropropylene) (PVDF-HFP)-based composite polymer electrolyte (CPE), designated as PPALx-D, is synthesized via a blade-casting method. This CPE comprises a conductive poly(poly(ethylene gly co l) methyl ether methacrylate-co-(lithium 2-acrylamido-2-methylpropanesulfonic acid)) (P(PEGMEMA-co-AMPSLi)) matrix, inorganic LATP filler, and an in-situ polymerized 1,3-dioxolane (DOL) artificial interlayer. The physicochemical and electrochemical properties of the as-prepared CPEs are systematically characterized. Results show that the PPAL5-D CPE, despite being thinner and containing less liquid electrolyte, provides faster organic-inorganic Li + transport channels and exhibits superior electrochemical compatibility with Li metal anodes. The PPAL5-D CPE achieves a high room-temperature (RT) ionic conductivity of 3.47× 10 −4 S cm −1 and a high Li + transference number of 0.61. The assembled LFP|PPAL5-D|Li battery demonstrates significantly improved cycling stability, delivering a discharge capacity of 131.5 mAh g −1 at 1C for 400 cycles at RT. This study proposes a feasible methodology for preparing organic-inorganic composite electrolytes, advancing the development of quasi-solid-state Li metal batteries (LMBs).
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Changwei Luo,Guoqiang Zhao,Mengyang Zhang,Bin Wu,Qingsong Hua
NASICON-type Li1.3Al0.3Ti1.7(PO4)3 (LATP) is a widely used solid electrolyte in solid-state lithium batteries, owing to its excellent chemical stability against moisture and high total ionic conductivity. However, traditionally, densification of LATP has been achieved through a high-temperature sintering process (approximately 1000 °C) owing to its poor sinterability. Herein, we report a facile synthesis route to obtain highly sinterable LATP solid electrolyte using tetrabutyl titanate (C16H36O4Ti) as the titanium source and incorporating the traditional solid-state reaction method. The synthetic LATP powder mixed with a low ratio of LiTiPO5 exhibited a hybrid crystalline–amorphous phase structure, which facilitated grain fusion, promoted structural homogeneity, and facilitated structural densification under low-temperature sintering. The sintered LATP pellet, which exhibited an interconnected structure and indistinct grain boundaries, achieved a relative density of >90% and an ionic conductivity of 0.667 mS/cm at a sintering temperature of only 750 °C. Additionally, we systematically studied and demonstrated the synthesis reaction mechanism, sintering behavior, and ionic diffusion kinetics of LATP electrolytes. Our study paves the way for synthesizing highly sinterable LATP solid electrolytes using a simple, additive-free, and cost-effective method.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 46
·2305326
·
IF 13.3
Shida Xue,Shiming Chen,Yanda Fu,Hengyao Zhu,Yuchen Ji,Yongli Song,Feng Pan,Luyi Yang
Composite solid electrolytes (CSEs) consisting of polyethylene oxide (PEO) matrix and active inorganic fillers have shown great potential for practical applications. However, mechanisms of how different active fillers enhance ion transport in CSEs still remain inconclusive. In this work, the component dependencies of ionic conductivity of PEO-based CSEs are investigated by comparing two widely investigated active fillers: NASICON-type (LATP) and garnet-type (LLZTO). In terms of ionic conductivity, the optimum ratios are strikingly different for LLZTO (10 wt%) and LATP (50 wt%). Through experimental and computational studies, it is demonstrated that the high affinity between LATP and PEO facilitates unhindered interfacial Li + transfer so that LATP functions as a bulk-active filler to provide additional inorganic ion pathways. By contrast, Li + transfer between LLZTO and PEO is found to be sluggish. Instead, LLZTO mainly improves ionic conductivity by dissociating lithium salt, making it a surface-active filler. Through categorizing active fillers based on their Li + conductive mechanisms, this work provides new understanding and guidelines for componential design and optimization of solid composite electrolytes.
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 COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiangming Cui,Xin Chen,Changzheng Lin,Jingzhao Wang,Zirui Guo,Mi Zhou,Zhouzhou Yao,Jiaxin Zhang,Shiyi Sun,Jianan Wang,Wei Yan
The advancement of high-energy–density and intrinsically safe all-solid-state lithium metal batteries (ASSLMBs) is crucial for the comprehensive electrification of energy consumption. Nevertheless, intrinsic defects in solid-state electrolytes (SSEs) and suboptimal interfacial contacts often lead to uncontrolled dendritic growth during practical battery operation. To address these challenges, this study proposes an integrated optimization strategy for bulk-phase defects and interfacial contacts of Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) SSEs based on ultra-fast Joule heating sintering (UHS) technique. Introducing specific sintering auxiliaries and a dual-process sintering approach can achieve the rapid densification of LATP SSEs. Additionally, the thermal pulse welding (TPW) technique for the integrated anode/SSE/cathode further provides superior SSE/electrode interface contact, facilitating the in-situ formation of a continuous ion-conducting network for improved electrochemical kinetics. The optimized Li||LATP||NCM811 ASSLMBs demonstrate exceptional specific capacity (185.9 mAh/g at 0.2 C) and robust cycling stability (90.9 % capacity retention after 100 cycles). This integrated optimization strategy can offer a critical technical reference for the rapid fabrication of high-performance ASSLMBs.
研究领域:
材料科学
·
电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Lifan Wang,Danya Gong,Siheng Niu,Leiying Wang,Qinling Shi,Xindong Wang,Jinli Qiao,Guicheng Liu,Chun Zhan
Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP)-based all-solid-state lithium battery (ASSLB) assembled with Ni-rich layered cathode (NCM), of much interest because of its high energy–density and safety, presents many challenges, one of which is poor interfacial instability resulting in large interfacial resistance. Nevertheless, the mechanism of electrochemical side reactions on the interfacial deterioration hasn’t been much investigated specifically, despite their close relationships in electrochemical performance. Herein, we report that the fundamental origin of interfacial chemical reactions is the migration of Ni 2+ from the nickel-rich cathodes to the NCM/LATP interface, for the first time, and the simultaneous chemical reaction with Ti 4+ in LATP, followed by the decomposition of LATP. In view of this, an elaborately designed regulation strategy, in-situ construction of the layered perovskite La 4 NiLiO 8 buffer layer , is proposed to effectively reduce the content of Ni 2+ on the surface of the nickel-rich cathodes and alleviate the chemical reaction between Ni 2+ and Ti 4+ , thereby improving the interfacial stability between NCM and LATP. As a result, the assembled ASSLBs with the La 4 NiLiO 8 buffer layer exhibit high initial discharge capacity (171.49 mAh/g) and excellent cycling performance with 89.47 % capacity retention after 100 cycles at 0.1C.
研究领域:
材料科学
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电化学
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能源存储技术
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Xianli Song,Haitao Zhang,Danfeng Jiang,Lipeng Yang,Jiahe Zhang,Meng Yao,Xiaoyan Ji,Gongying Wang,Suojiang Zhang
Solid-state batteries , which exhibit characteristics including uniform Li deposition, non-flammability and low interfacial resistance, are desirable for novel energy storage devices. Herein, a self-standing, fireproof and electrochemically stable organic-inorganic composite ionogel electrolyte was carefully designed and prepared by using polymerized ionic liquid (PIL), ionic liquid (IL), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and lithium aluminum titanium phosphate (LATP) nanoparticles . The incorporation of LATP nanoparticles into polymer backbone was found to facilitate ionic transport due to the homogenous Li + distribution, which would further boost the ionic conductivity and mechanical properties. In addition, the introduction of IL favored the reduction of interface resistance. Benefiting from the nonflammability, the thermal shrinkage performance of as-prepared electrolyte could stand over a broad operating temperature range. A Li/Li symmetric cell containing optimized PIL-14 wt% LATP could be cycled steadily for over 2000 h at 50 °C. A lithium metal battery containing composite ionogel electrolyte exhibited an outstanding specific capacity of 145 mAh g −1 and 95% capacity retention at 50 °C even after 100 cycles. This study indicates that the co-employment of IL and inorganic nanoparticle is an effective strategy for the construction of organic-inorganic hybrid electrolytes for high-safety solid-state lithium metal batteries (LMBs).
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2025
·Vol. 31
·期 12
·e202403915
·
IF 3.7
Qi Pan,Wanliang Yang,Chen Wu,Dongjia Xie,Yuan Wang
Graphical A ploy(1,3-dioxolane) (PDOL) layer was constructed by a Al(OTf) 3 -induced in-situ solidification process between the interface of LATP and anode/cathode. The as-prepared PDOL as an “interfacial adhesive” can fill the gap between the LATP and the electrode, providing a better interfacial contact and reduced interfacial impedance. Such interfacial adhesive layer not only effectively prevents Li metal from reducing LATP but also provides intimate interface contact and limits unnecessary electron transport. Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) as the solid-electrolyte has attracted much attention for Li-ion batteries. However, the unstable LATP/Li interface and the insufficient contact between the anode/cathode and LATP usually lead to the structural collapse of LATP and the large solid–solid interfacial resistance for Li+ transport. Herein, a poly(1,3-dioxolane) (PDOL) adhesive layer was constructed by a Al(OTf) 3 -induced in-situ solidification process between the interface of LATP and anode/cathode. Such PDOL interfacial adhesive layer alleviates adverse reduction reactions at the LATP/Li interface and provides stable and well-contacted bilateral electrode interfaces. Benefitting from the PDOL interfacial adhesive, the Li|adhesive-LATP|Li symmetric cells achieve a current density up to 0.7 mA cm −2 and exhibit a good cycling stability for more than 2750 h at 0.1 mA cm −2 , and the Li|adhesive-LATP|LiFePO4 solid-state batteries with interface modification exhibit a capacity of 158 mAh g −1 at 0.2 C with a retention of 94 % after 100 cycles.
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
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Jingrui Kang,Rui Gu,Xu Guo,Jing Li,Hongchen Sun,Leiyang Zhang,Ruiyi Jing,Li Jin,Xiaoyong Wei
NASICON-type structured compounds Li 1+ x M x Ti 2- x (PO 4 ) 3 (M = Al, Fe, Y, etc.) have captured much attention due to their air stability, wide electrochemical window and high lithium ion conductivity. Especially, Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) is a potential solid electrolyte due to its high ionic conductivity . However, its actual density usually has a certain gap with the theoretical density, leading the poor ionic conductivity of LATP. Herein, LATP solid electrolyte with series of SnO–P 2 O 5 –MgO (SPM, 0.4 wt%, 0.7 wt%, 1.0 wt%, 1.3 wt%) glass addition was successfully synthesized to improve the density and ionic conductivity. The SPM addition change Al/Ti–O bond and P–O bond distances, leading to gradual shrinkage of octahedral AlO 6 and tetrahedral PO 4 . The bulk conductivity of the samples increases gradually with SPM glass addition from 0.4 wt% to 1.3 wt%. Both SPM and the second-phase LiTiPO 5 , caused by glass addition, are conducive to the improvement of compactness. The relative density of LATP samples increases first from 0 wt% to 0.7 wt%, and then decreases from 0.7 wt% to 1.3 wt% with SPM glass addition. The grain boundary conductivity also changes accordingly. Especially, the highest ionic conductivity of 2.45 × 10 −4 S cm −1 , and a relative density of 96.72% with a low activation energy of 0.34 eV is obtained in LATP with 0.7 wt% SPM. Increasing the density of LATP solid electrolyte is crucial to improve the ionic conductivity of electrolytes and SPM glass addition can promote the development of dense oxide ceramic electrolytes.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
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 THE AMERICAN CERAMIC SOCIETY
·
2023
·Vol. 107
·期 4
·2407-2420
·
IF 3.9
Xiaojuan Lu,Ziqian Li,Songtao Liu,Ke Huang,Jiankang Hai
Rare earth elements (Pr, Eu, Lu) with larger ionic radius and lower electronegativity were used to dope NASICON type solid electrolyte Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) by solid state method. The effects of the types and the doping amounts of rare earth elements on the properties of LATP were investigated systematically. A test cell of Li 4 Ti 5 O 12 //Lu-LATP//LiCoO 2 was assembled and the cycling performance was evaluated. The failure mechanism of the test cell was analyzed. The relative density, cell volumes, and the total ionic conductivity of LATP were increased upon doping of rare-earth elements. The grain sizes and the electronic conductivity were decreased. Among the three rare earth elements studied, Lu doped LATP achieved the highest total ionic conductivity of 3.6 × 10 4 S/cm, with the lowest activation energy of 0.23 ev, and the electronic conductivity was one order of magnitude lower than that of un-doped LATP. The enhancement of the total conductivity was ascribed to the synergized effect of the increase of the relative density, the enlargement of the cell volumes and the broadening of Li + migration window owing to the larger ionic radius and the lower electronegativity of the rare earth elements. Based on the relaxation time distribution spectra, the failure mechanism of the assembled cell was attributed to the degradation of the electrolytes and the irreversible decomposition of electrodes.
研究领域:
材料科学
·
电化学
·
储能
·
固体离子学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xuan Wang,Shuo Huang,Benben Wei,Min Liu,Bo Yang,Ruoqing Liu,Hongyun Jin
All-solid-state batteries with oxide electrolytes and high-nickel layered oxide cathodes (LiNixCoyMnzO2 and LiNixCoyAlzO2, x + y + z = 1, x ≥ 60%) have received widespread attention owing to their high energy density and high safety. However, they generally suffer from interfacial structural instability when coupled with solid-state electrolytes, which strongly diminishes the longevity of the battery. In this work, we propose adding a sacrificial additive C60 to the catholyte buffer layer between Li1.4Al0.4Ti1.6(PO4)3 (LATP) and LiNi0.8Co0.1Mn0.1O2 (NCM811) to enhance the electrochemical stability under high-voltage operating conditions. A uniform and robust cathode–electrolyte interphase (CEI) film enriched with LixPOyFz, LiPxFy, and C60Fn is spontaneously formed on the surface of the cathode particles. In addition, the NCM811/Li solid-state battery delivers a discharge capacity of 150.3 mAh g–1 with a retention of 85% after 200 charge–discharge cycles at 0.5 C. This study offers a practical approach toward realizing LATP-based all-solid-state high-voltage batteries characterized by exceptional cycling stability.
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
危险品化学品经营许可证（带存储）