ACS Applied Materials & Interfaces
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2024
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IF 8.3
Rundi Xiong,Lixia Yuan,Ruifeng Song,Shuaipeng Hao,Haijin Ji,Zexiao Cheng,Yi Zhang,Bowen Jiang,Yudi Shao,Zhen Li,Yunhui Huang
Superionic halides have attracted widespread attention as solid electrolytes due to their excellent ionic conductivity, soft texture, and stability toward high-voltage electrode materials. Among them, Li3InCl6 has aroused interest since it can be easily synthesized in water or ethanol. However, investigations into the influence of solvents on both the crystal structure and properties remain unexplored. In this work, Li3InCl6 is synthesized by three different solvents: water, ethanol, and water–ethanol mixture, and the difference in properties has been studied. The results show that the product obtained by the ethanol solvent demonstrates the largest unit cell parameters with more vacancies, which tend to crystallize on the (131) plane and provide the 3D isotropic network migration for lithium-ions. Thus, it exhibits the highest ionic conductivity (1.06 mS cm–1) at room temperature and the lowest binding energy (0.272 eV). The assembled all-solid-state lithium metal batteries (ASSLMBs) employing Li3InCl6 electrolytes demonstrate a high initial discharge capacity of 153.9 mA h g–1 at 0.1 C (1 C = 170 mA h g–1) and the reversible capacity retention rate can reach 82.83% after 50 cycles. This work studies the difference in ionic conductivity between Li3InCl6 electrolytes synthesized by different solvents, which can provide a reference for the future synthesis of halide electrolytes and enable their practical application in halide-based ASSLMBs with a high energy density.
研究领域:
材料科学
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电化学
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能源存储与转换
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
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IF 5.6
Chen Liu,Siwu Li,Lin Li,Qiyue Luo,Liang Ming,Ziling Jiang,Ziyu Lu,Miao Deng,Jie Yang,Shijie Cheng,Chuang Yu
The sulfide electrolyte-based all-solid-state batteries with high-nickel layered oxide cathodes face significant challenges due to the narrow electrochemical window of sulfides and severe side reactions caused by direct contact with high-voltage oxide cathode materials such as LiNi 0.9 Mn 0.05 Co 0.05 O 2 (NCM90). Here, we successfully synthesized Li 3 InCl 6 (LIC) halide electrolytes through ball-milling followed by annealing method, achieving the ionic conductivity of 2.0 mS cm −1 at room-temperature. The interface between this electrolyte and NCM90 cathode material without any interface modification is stable. By introducing the LIC electrolyte layer, the NCM90/LIC+Cl1.5/Li-In battery exhibits significantly improved electrochemical performance at different temperatures, particularly in terms of initial discharge capacity. Notably, the battery demonstrates outstanding discharge capacity and cycling stability at low temperatures. Experimental investigations reveal that the introduction of the LIC electrolyte with high oxidation potential facilitates the H2-H3 phase transition in NCM90 during high-voltage operation, which is critical for enhancing the discharge capacity. This work provides fundamental insights into interfacial engineering strategies for high-voltage sulfide-based all-solid-state battery systems.
研究领域:
储能
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材料科学
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电化学
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固态电池技术
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产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2026
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IF 3.1
Sun Shuze,Ma Xuefang,Wang Qingtao
Halide solid electrolytes have emerged as highly attractive electrolyte materials owing to their excellent ionic conductivity and high oxidation potential. In this work, low-cost CuCl is employed as a dopant, and Cu⁺-doped Li₃InCl₆ is prepared via ball milling, yielding a series of novel Li₃₋ ₓ Cu ₓ InCl₆ (0 ≤ x ≤ 0.4) electrolytes. Cu⁺ doping modifies the crystal structure and regulates the ionic conductivity of the material. Among them, Li₂.₉Cu₀.₁InCl₆ exhibits a lower activation energy and achieves a room-temperature ionic conductivity of 1.04 mS cm⁻¹. Cu⁺ doping enhances the air stability of Li₃InCl₆ and mitigates the degradation of ionic conductivity after air exposure. Furthermore, Cu⁺ doping reduces surface cracks, improves the deformability of the material, and lowers interfacial resistance. All-solid-state batteries using Li₂.₉Cu₀.₁InCl₆ as the electrolyte display superior capacity and cycling performance compared to those with pristine Li₃InCl₆. This work demonstrates that Cu⁺ doping is an effective strategy to boost ionic conductivity, improve air stability, and enhance the electrochemical performance of Li₃InCl₆.
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DOI
高影响因子
Journal of Energy Storage
·
2026
·
IF 9.8
Bo Li,Lei Xian,Fu-Jie Zhao,Zu-Tao Pan,Ling-Bin Kong
Solid electrolytes, as the core components of all-solid-state batteries, are a prominent research focus due to its lithium-ion rapid diffusion capability. The halide solid electrolyte Li 3 InCl 6 , distinguished by its high ionic conductivity and remarkable moisture reversibility, has garnered considerable attention in the realm of electrochemistry. This study systematically investigates the influence of Li + vacancy defect concentration on lattice configuration and ionic transport properties through In-rich compositional modulation in Li 3 InCl 6 electrolytes with varying Li/In cation ratios. Experimental results reveal that, under an invariant primary lattice framework, increasing In 3+ content induces preferential occupation of the 4 g Wyckoff sites by In 3+ , generating lattice distortion that deforms the cation layer in the (001) crystallographic plane. Concurrently, substantial tetrahedral vacancy defects emerge within the Li + layer of the (002) plane. This synergistic structural evolution markedly enhances lithium-ion transport kinetics by weakening anion framework constraints on Li + migration. Correspondingly, electrochemical characterization demonstrates that the optimized Li 2.55 In 1.15 Cl 6 electrolyte achieves a threefold increase in ionic conductivity compared to the pristine sample. The performance enhancement originates from distorted non-migrating ion sites and generated vacancy defects within the crystal lattice. Consequently, all-solid-state lithium batteries incorporating this optimized electrolyte exhibit significantly improved cycling stability and rate capability. This study prepares Li 3-3x In 1+x Cl 6 via ball milling and investigates the structure-performance relationships through vacancy regulation, demonstrating a viable strategy for solid-state electrolyte design.
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2022
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IF 10.383
Xuming Luo,Dan Cai,Xiuli Wang,Xinhui Xia,Changdong Gu,Jiangping Tu
Halide electrolytes are rising stars among inorganic solid-state electrolytes due to their high ionic conductivity and good compatibility with high-voltage electrodes. However, their traditional synthesis methods including ball-milling annealing are usually energy-intensive and time-consuming compared with liquid-mediated routes. What’s more, the only method in aqueous solution is not perfect considering detrimental effect of trace water for battery performances. Here, we propose a novel ethanol-mediated synthesis route for superionic Li3InCl6 electrolyte via energy-friendly dissolution and post-treatment. The organics in ethanol-mediated precursor disappear in form of light gas during post-treatment. And Li3InCl6 with best thermal stability and ionic conductivity (0.79 mS cm–1, 20 °C) can be successfully prepared after postheating for 3 h at 200 °C. Besides, it is also found that the ionic conductivity of Li3InCl6 is positively correlated with peak intensity ratio of (131) plane/(001) plane since crystal plane and preferred orientation can directly affect polyhedrons through which lithium ions migrate in crystalline conductors. The assembled LiNi0.8Co0.1Mn0.1O2/Li3InCl6/Li10GeP2S12/Li–In cell presents high initial charge capacity of 174.8 mAh g–1 at 0.05 C and a good rate performance of 122.9 mAh g–1 at 1 C. Especially, the retention rate of charge capacity can reach 94.8% after 200 cycles. The ethanol-mediated synthesized Li3InCl6 is a novel promising electrolyte which can be coupled with high-voltage cathode for the application of all-solid-state lithium-metal batteries.
研究领域:
材料科学
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电化学
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能源存储
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2026
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IF 9.2
Weiye Ma,Lun Zhang,Guanghan Zhu,Hongrui Kang,Haiyang Yuan,Yongyi Long,Zhiyi Pan,Zhiqiang Liu,Xiaojing Liu,Jin Liang,Yuxin Liang,Zhenduo Cui,Shengli Zhu,Ying Zhao,Zhonghui Gao
Poly(ethylene oxide) (PEO)-based electrolytes are promising for all-solid-state batteries but are typically limited to elevated temperatures due to PEO crystallinity and strong Li⁺–EO coordination. Here, we report a homogeneous PEO–LiTFSI electrolyte incorporating optimized Li3InCl6 that suppresses PEO crystallization, weakens Li⁺–TFSI⁻ coordination, and enhances Li-ion transport after acetonitrile solvent removal. This effect originates from the structural collapse of Li3InCl6 in acetonitrile, which exposes In3⁺ sites that preferentially adsorb TFSI⁻ anions, thereby disrupting the regular arrangement of PEO chains and inducing amorphization. In contrast to other oxide-based inorganic fillers, our results also found that the interface between PEO and Li3InCl6 enables efficient Li-ion transport. The resulting electrolyte achieves a high room-temperature ionic conductivity of 1.13×10⁻4 S cm-1 and excellent cycling stability with a LiNi0.8Co0.1Mn0.1O2 cathode, retaining 74 % capacity after 100 cycles at 0.3 C and 25 oC. To confirm the generality of this strategy and mechanism, we extended it to InCl3 and GaCl3 fillers, which similarly promoted amorphization in PEO–LiTFSI electrolytes. This work provides a general strategy to design amorphous polymer electrolytes for high-voltage solid-state batteries operating at room temperature.
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DOI
高影响因子
Applied Materials Today
·
2023
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IF 8.3
Chaochao Wei,Shaoqing Chen,Chuang Yu,Ru Wang,Qiyue Luo,Shuai Chen,Zhongkai Wu,Chongxuan Liu,Shijie Cheng,Jia Xie
Sb-based lithium sulfide electrolytes are promising for all-solid-state lithium battery applications due to their ultrahigh Li-ion conductivity (10 −2 S/cm) which is even comparable to current liquid electrolytes. However, the poor electrochemical stability between this electrolyte and high voltage layered structure cathode makes it difficult to achieve excellent battery performances. Herein, Li 6.5 Sb 0.5 Ge 0.5 S 5 I electrolyte with ionic conductivity up to 10 m S/cm is successfully synthesized and the electrochemical failure mechanism of the corresponding battery using bare LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathode and Li-In anode is revealed. Furthermore, Li 3 InCl 6 electrolyte is introduced both as an ionic additive in the cathode mixture and as an isolating layer to avoid side reactions. The designed configuration delivers a high discharge capacity of 162.7 mAh/g at 0.5C and sustains 74.5% of the capacity after 200 cycles at room temperature. Moreover, it also can reversibly cycle from -20 to 60 °C with superior battery performances. This work provides a general design strategy for utilizing highly conductive sulfide electrolytes with low stability in all-solid-state batteries.
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Qing Ye,Xiaohan Li,Wenkui Zhang,Yang Xia,Xinping He,Hui Huang,Yongping Gan,Xinhui Xia,Jun Zhang
The implementation of all-solid-state lithium batteries (ASSLBs) is regarded as an important step toward the next-generation energy storage systems. The sulfide solid-state electrolyte (SSE) is a promising candidate for ASSLBs due to its high ionic conductivity and easy processability. However, the interface stability of sulfide SSEs toward high-capacity cathodes like nickel-rich layered cathodes is limited by the interfacial side reaction and narrow electrochemical window of the electrolyte. Herein, we propose introducing the halide SSE Li3InCl6 (LIC) with high (electro)chemical stability and superior Li+ conductivity to act as an ionic conductive additive in the Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM) cathode mixture through a slurry coating, aiming to build a stable cathode–electrolyte interface. This work demonstrates that the sulfide SSE Li5.5PS4.5Cl1.5 (LPSCl) is chemically incompatible with the NCM cathode, and the indispensable role of the substitution of LPSCl with LIC in enhancing the interfacial compatibility and oxidation stability of the electrolyte is highlighted. Accordingly, this new configuration shows superior electrochemical performance at room temperature. It shows a high initial discharge capacity (136.3 mA h g–1 at 0.1C), cycling performance (77.4% capacity retention at the 100th cycle), and rate capability (79.3 mA h g–1 at 0.5C). This work paves the way for investigating interfacial challenges regarding high-voltage cathodes and provides new insights into possible interface engineering strategies.
研究领域:
材料科学
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电化学
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储能技术
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固态电池
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界面工程
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Xiaohan Li,Qing Ye,Zhan Wu,Wenkui Zhang,Hui Huang,Yang Xia,Yongping Gan,Xinping He,Xinhui Xia,Jun Zhang
The all-solid-state lithium battery (ASSLB) with lithium-rich manganese oxide (LRMO) cathode material is one of the strongest competitors for the next generation energy-storage device with high energy density. However, due to the serious interfacial reaction between LRMO and halide solid-state electrolyte (SSE), its electrochemical performance cannot meet the practical demand. In this work, in-situ electrochemical impedance spectroscopy (EIS), X-ray photoelectron spectroscopy (XPS) tests and high resolution transmission electron microscope (HR-TEM) are carried out to clarify the interfacial reaction mechanism between LRMO and Li 3 InCl 6 (LIC). The active oxygen released from LRMO and phase transition of LRMO are confirmed to seriously deteriorate the LRMO/LIC interface. To solve the above problems, a uniform LiNbO 3 coating is introduced to alleviate the interfacial side reaction and phase transition of LRMO. With moderate coating amount (1.5 wt%, ∼10 nm thick), the LNO@LRMO cathode shows an initial discharge capacity of 185 mA h g − 1 with 67% capacity retention after 100 cycles in halide-based ASSLB, which greatly exceeds that of bare LRMO cathode under voltage range of 2.3–4.8 V. This work provides a new perspective for improving the performance of LRMO in halide-based ASSLBs to achieve high energy density.
研究领域:
材料科学
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电化学
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能源存储
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固态离子学
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先进电池技术
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2026
·
IF 10.7
Junming Han,Chunbo Guo,Fangyu Hao,Zihao Cai,Hao Zheng,Zeyi Jiang,Nien-Chu Lai
A high-purity Li 3 InCl 6 electrolyte is synthesized via a facile room-temperature liquid-phase method. • Nb 5+ doping induces lattice distortion and increases lithium vacancy concentration. • The Nb-Doped electrolyte achieves a high ionic conductivity and excellent electrochemical stability. • The assembled all-solid-state lithium battery delivers superior rate capability and long cycling life. Halide solid electrolytes hold great promise for all-solid-state lithium batteries (ASSLBs), yet achieving fast Li + transport and high electrochemical stability through scalable synthesis remains challenging. Herein, we report a facile wet-chemical route to synthesize Nb-doped Li 3 InCl 6 solid electrolytes, where a stepwise slow drying and thermal treatment protocol is adopted to regulate crystallization kinetics. By optimizing the solvent and dopant concentration, the 10% Nb-substituted sample (LIC Nb 1 ) prepared in ethanol shows optimal performance. Structural refinement and spectroscopic analysis reveal that aliovalent Nb 5+ creates Li vacancies and optimizes local lattice environments, promoting fast Li + conduction. Accordingly, LIC-Nb 1 exhibits a room-temperature ionic conductivity of 0.95 mS cm −1 , more than twice that of pristine LIC(Et) (0.44 mS cm −1 ), with a lower activation energy of 0.31 eV and enhanced electrochemical stability. ASSLBs based on LIC-Nb 1 delivers substantially improved rate capability and cycling stability relative to pristine LIC-based cells. At 30 °C, the LIC-Nb 1 -based cell shows stable charge/discharge behavior over 2–4.4 V (vs. Li/Li + ), affording an initial discharge capacity of 182.4 mAh g −1 , and an initial Coulombic efficiency of 91.02%. Under the more demanding rate and prolonged cycling evaluations conducted at 60 °C, the capacity retention of LIC-Nb 1 -based cell after 30 cycles at 0.1C under 100% depth of discharge reaches 83.5%, compared with 66.8% for the LIC(Et)-based counterpart. This work systematically clarifies the solvent effect on the crystal structure and ionic conductivity of LIC electrolytes, proposes a crystallization kinetics modulation strategy to eliminate structural defects, and validates the practical application potential of Nb-doped LIC electrolytes in high-voltage ASSLBs. These findings highlight the integrated strategy of kinetic regulation and heteroatom doping as an effective strategy for engineering high-performance halide solid electrolytes toward advanced all-solid-state lithium batteries. Download: Download high-res image (226KB) Download: Download full-size image
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2023
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IF 9.2
Chengjin Liu,Chang Miao,Manyi He,Jiale Wang,Qiyan Chen,Shuqing Nie,Wei Xiao
LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) powders modified with fast ion conductor Li 3 InCl 6 (LIC) are fabricated via sol-gel and sintering processes, and the LIC layer with a thickness of about 2.4842 nm is uniformly covered on the surface to fabricate the targeted LIC@NCM523-2 composite powders , in which the LIC layer not only lowers the residual lithium content but also decreases the cation mixing degree. The LIC@NCM523-2 electrode preserves relatively intact morphology and layered structure after cycles. Moreover, the LIC@NCM523-2 electrode delivers discharge specific capacity of 130.5 mAh g −1 with capacity retention ratio of 76.8% after 200 cycles at 1.0 C and 25 °C, and retains about 108.8 mAh g −1 at the 200th cycle at 1.0 C and 60 °C. Importantly, the LIC@NCM523-2 electrode exhibits desirable discharge specific capacity of 128.2 mAh g −1 at 5.0 C and easily returns back to 164.3 mAh g −1 at 0.1 C and 25 °C. Those outstanding electrochemical properties are ascribed to the fact that the appropriate thickness LIC layer protects active particles from the corrosion of liquid electrolytes to stabilize the internal structure and provides high conductivity to facilitate Li + ions transport, elucidating the importance of the surface modified strategy with the fast ion conductor LIC layer.
研究领域:
材料科学
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能源存储技术
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Qian Zhao,Weizong Wang,Cheng Ruan,Zhengping Ding,Peng Wei,Xiangqun Zhuge,Yurong Ren
Developing advanced halide solid-state electrolytes (SSEs) with both high ionic conductivity and high-voltage stability is crucial for high-energy all-solid-state batteries (ASSBs). However, conventional strategies such as simple cation substitution or anion engineering for achieving these properties simultaneously often require compromising one for the other. Herein, a high-entropy strategy is employed to design and synthesize Li3–4xIn1–6xFexYxZr2xHf2xCl6 (0 ≤ x ≤ 0.05) through multication substitution in Li3InCl6 (LIC). Li2.92In0.88Fe0.02Y0.02Zr0.04Hf0.04Cl6 (HE-LIC) featuring moderate lattice distortion achieves the highest ionic conductivity of 1.136 mS cm–1 at 25 °C and improved high-voltage stability. Based on theoretical calculations and experimental findings, the tailored distortion elongates Li1–Cl bonds (2.6616 vs 2.6531 Å in LIC) to facilitate Li+ conduction, while confining Cl– distribution to inhibit oxidation. ASSBs with HE-LIC and LiCoO2 cathode deliver a discharge capacity of 151.13 mAh g–1 and 81.17% capacity retention after 100 cycles at 0.5 C under 4.5 V. Even at 4.6 V, a discharge capacity of 165.98 mAh g–1 with 80.63% retention after 50 cycles at 0.5 C is achieved. These findings demonstrate the potential of high-entropy-driven moderate lattice distortion for advanced SSEs in high-voltage ASSBs.
研究领域:
材料科学
·
储能技术
·
固态离子学
·
电池技术
✓ 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）