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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Flexible and freestanding heterostructures based on COF-derived N-doped porous carbon and two-dimensional MXene for all-solid-state lithium-sulfur batteries

Yuchan Zhang,Yang Wu,Yongpeng Liu,Jinkui Feng

Lithium-sulfur (Li-S) batteries are considered as one of the best future profession power sources owing to their ultrahigh energy density. Nevertheless, the commercialized Li-S batteries is challenging owing to the shuttle effect of lithium polysulfides (LiPSs), poor electronic activity of sulfur and safety issues. In this work, flexible and binder-free 3D porous 1,3,5-triformylbenzene-tris(4-aminophenyl) amine (Tf-TAPA) covalent-organic framework (COF) derived N-doped carbon (CTT)/ 2D transition metal carbides and nitrides (MXene) paper is designed as electronic conductive sulfur host to restrict the LiPSs. To boost the safety of Li-S batteries and further reduce the LiPSs diffusion, all-solid-state Li-S batteries are constructed by utilizing polyethylene oxide (PEO)-based solid electrolyte with low LiPSs solubility and high safety. With the synergistic advantages of porous and electronic conductive CTT, MXene and solid-state electrolyte, the all-solid-state Li-S batteries display excellent safety character and stable cycling stability about 584 mAh g −1 even after 100 cycles.

研究领域: 材料科学 · 能源存储
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ACS Nano · 2024 · IF 15.8

Dendrite-Free All-Solid-State Lithium Metal Batteries by In Situ Phase Transformation of the Soft Carbon–Li3N Interface Layer

Ming Yang,Kaiqi Yang,Yujing Wu,Zhixuan Wang,Tenghuan Ma,Dengxu Wu,Li Yang,Jieru Xu,Pushun Lu,Jian Peng,Zhiwen Jiang,Xiang Zhu,Qifa Gao,Fuqiang Xu,Liquan Chen,Hong Li,Fan Wu

The accelerated formation of lithium dendrites has considerably impeded the advancement and practical deployment of all-solid-state lithium metal batteries (ASSLMBs). In this study, a soft carbon (SC)–Li3N interface layer was developed with both ionic and electronic conductivity, for which the in situ lithiation reaction not only lithiated SC into LiC6 with good electronic/ionic conductivity but also successfully transformed the mixed-phase Li3N into pure-phase β-Li3N with a high ionic conductivity/ion diffusion coefficient and stability to lithium metal. The mixed conductive interface layer facilitates fast Li+ transport at the interface and induces the homogeneous deposition of lithium metal inside it. This effectively inhibits the formation of lithium dendrites and greatly improves the performance of the ASSLMB. The ASSLMB assembled with the SC–Li3N interface layer exhibits high areal capacity (15 mA h cm–2), high current density (7.5 mA cm–2), and long cycle life (6000 cycles). These results indicate that this interface layer has great potential for practical applications in high-energy-density ASSLMBs.

研究领域: 材料科学 · 电化学 · 能源存储
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

Solid polymer electrolytes incorporating cubic Li7La3Zr2O12 for all-solid-state lithium rechargeable batteries

Fei Chen,Dunjie Yang,Wenping Zha,Bodi Zhu,Yanhua Zhang,Junyang Li,Yuping Gu,Qiang Shen,Lianmeng Zhang,Donald R. Sadoway

The advantages of all-solid-state batteries in terms of high energy density and improved safety have accelerated the research into durable and reliable solid electrolytes and into scale up of their processing technology. High lithium-ion-conducting Li 7 La 3 Zr 2 O 12 (LLZO) ceramic-based solid electrolytes have been intensively studied recently, but their widespread commercial deployment has been constrained due to their fragility and brittleness . In the present study, LLZO ceramic powders have been successfully incorporated into the polyethylene oxide (PEO) polymer by tape casting. The ionic conductivity of the PEO/LLZO composite electrolyte membranes is significantly enhanced at the optimal LLZO concentration of 7.5 wt.% at which the materials exhibits maximum ionic conductivity of 5.5 × 10 −4  S·cm −1 at 30 °C. The ionic conductivity enhancement mechanism of the composite electrolyte is revealed by differential scanning calorimetry (DSC), which shows that the LLZO filler represses crystallinity in PEO. Furthermore, as evidence of the advantageous electrochemical properties of the composite electrolyte an all-solid-state battery of LiFePO 4 /Li fabricated herein delivered a maximum discharge capacity of 150.1 mAh·g −1 at 0.1C, good cycling performance, and excellent rate capability under 60 °C.

研究领域: 材料科学 · 电化学
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CHEMISTRY OF MATERIALS · 2023 · IF 8.6

Insight into the Extreme Side Reaction between LiNi0.5Co0.2Mn0.3O2 and Li1.3Al0.3Ti1.7(PO4)3 during Cosintering for All-Solid-State Batteries

Yaqi Chen,Xieyu Xu,Jianli Cheng,Xuyang Wang,Dawei Wang,Yongjing Wang,XingXing Jiao,Jian Chen,Shizhao Xiong,Zhongxiao Song,Yangyang Liu

All-solid-sate batteries (ASSBs) with a NASICON-type solid-state electrolyte (SSE) of Li1.3Al0.3Ti1.7(PO4)3 (LATP) can be accepted as a promising candidate to significantly improve safety and energy density due to their high oxidation potential and high ionic conductivity. However, thermodynamic instability between the cathode and LATP is scarcely investigated during cosintering preparation for the integrated configuration of ASSBs. Herein, the structural compatibility between commercially layered LiNi0.5Co0.2Mn0.3O2 (NCM523) and LATP SSE was systematically investigated by cosintering at 600 °C. It is noticeable that an extreme side reaction between Li from NCM523 and phosphate from LATP happens during its cosintering process, leading to a severe phase transition from a layered to a spinel structure with high Li/Ni mixing. Consequently, the capacity of NCM523 is lost during the preparation of the NCM523–LATP composite cathode. Based on this, we suggested that the interface modification of the NCM523/LATP interface is valued significantly to inhibit this extreme side reaction, quickening the application of LATP-based ASSBs.

研究领域: 材料科学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Enhancing Compatibility of Halide with Sulfide-Electrolytes via High Oxygen Incorporation for Robust Solid-State Batteries

Haochang Zhang,Pengcheng Yu,Ziang Cui,Hailun Jin,Wen Tang,Chunlei Zhao,Jiuwei Lei,Shuaika Liang,Zhepu Shi,Jianhui Wang,Ying Li,Fiaz Hussain,Jinlong Zhu,Wei Xia

Lithium-metal-halide (Li-M-X) solid-state electrolytes (SSEs) offer significant potential for high-energy-density all-solid-state batteries (ASSBs) due to their high ionic conductivity, deformability, and compatibility with cathodes. However, to prevent direct reactions between halide SSEs and reductive anodes, sulfide SSEs are commonly used as interlayers in ASSBs. Yet, the chemical and electrochemical incompatibilities between halides and sulfides pose a new challenge. Here, a dual-anion strategy is proposed and demonstrated to address this issue by introducing O 2− anions into the halide framework. These findings reveal that high-concentration oxygen incorporation in Zr-based halide SSEs can be achieved without compromising ion conductivity, while simultaneously reducing interfacial reaction energy with Li 6 PS 5 Cl sulfide SSEs. This results in the formation of a dense, low-resistance Li 3 PO 4 -enriched interfacial layer, which contributes to superior electrochemical performance in full cells. ASSBs utilizing this electrolyte pair and a high-loading LiCoO 2 cathode (19.3 mg cm −2 ) achieve an impressive areal capacity of 2.8 mAh cm −2 and stable cycling performance exceeding 400 cycles. The O/Cl dual-anion strategy is also applicable to other halide SSEs paired with representative sulfide SSEs, including Li 6 PS 5 Cl, Li 10 GeP 2 S 12 , Li 3 PS 4 , Li 7 P 3 S 11, and Li 6.7 SiSb 0.5 S 5 I. This work provides valuable insights and strategies to improve the compatibility between halide and sulfide SSEs, advancing the development of ASSBs.

研究领域: 材料科学 · 电化学 · 能源存储
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

A cyclic durable all-solid-state battery constructed with LiBH4-based electrolyte with high ionic conductivity at room temperature

Xueye Zhuang,Shiman He,Long Hu,Qian Shi,Hui Wang,Renzong Hu

LiBH 4 has been considered as a promising solid electrolyte for lithium-ion batteries. However, the low ionic conductivity at room temperature has been the biggest challenge of LiBH 4 solid-state electrolyte (SSE) toward practical solid-state batteries. In this work, a ternary electrolyte is designed and prepared by milling LiBH 4 with LiNH 2 and interfacially decorated with g-C 3 N 4 . It is revealed that the soft dispersed phase of two-dimensional g-C 3 N 4 can build an effective transportation network in the composite electrolyte, thereby decreasing the interfacial impedance and reducing the energy barrier for lithium ion diffusion. The optimized SSE, LiBH 4 -2LiNH 2 -g-C 3 N 4 -10 % (LBN-CN-10 %), exhibits an ionic conductivity of 1.5×10 −3 S cm −1 , five orders of magnitude higher than that of the LiBH 4 electrolyte at 30 °C. The LiIn symmetric cell with LBN-CN-10 % electrolyte delivers a low polarization of ∼89 mV over 10,000 h. When assembling with Li 4 Ti 5 O 12 cathode, the all-solid-state battery exhibits excellent cycling over 1000 cycles at 30 ℃, achieving a breakthrough in the lifetime of solid-state batteries with LiBH 4 -based electrolyte. Moreover, the all-solid-state battery with LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathode also delivers a discharge plateau at 3.0 V, revealing the high voltage withstanding of LBN-CN-10 % electrolyte. This work provides new options for the development and practical application of room-temperature hydride all-solid-state batteries.

研究领域: 材料科学 · 能源存储技术
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SOLID STATE IONICS · 2025 · IF 3.3

The effect of Ga doping on the microstructure and electrochemical properties of Li7La3Zr2O12 garnet-type solid electrolyte

Shihao Fu,Pingmei Li,Shiyu Yu,Yang Hu,Yibo Liu,Daming Chen,Yaqing Wei,Yuanxun Li,Yong Chen

The garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) has garnered significant attention due to its superior thermal stability and broad electrochemical window. However, LLZO exhibits instability at room temperature and readily transforms from a cubic phase ( c -LLZO) to a tetragonal phase ( t -LLZO), resulting in issues such as low ionic conductivity. Herein, the effect of Ga doping on LLZO is investigated. Combined with SEM, activation energy, ionic conductivity and XRD refinement, the results demonstrate that Li 7-3x Ga x La 3 Zr 2 O 12 exhibits better properties when x = 0.25. Solid-state nuclear magnetic resonance (SSNMR) showed that Ga0.25-LLZO was favorable for promoting Li + transport. Moreover, Li| [email protected] |Li symmetric cells exhibit lower interfacial specific impedance (IASR) and higher critical current density (CCD) than both Li|Ag@Ga0-LLZO|Li and Li| [email protected] |Li and was stabilized at 0.15 mA/cm 2 for 1300 h of stable cycling. In addition, the all-solid-state battery Li| [email protected] |LFP was cycled at 0.2C for 100 cycles with 82 % capacity retention, demonstrating its promising application in lithium batteries.

CAS / MDL: 1344-28-1
研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2023 · IF 6.4

Stabilized Cathode/Sulfide Electrolyte Interface through Conformally Interfacial Nanocoating for All-Solid-State Batteries

Changfei Zou,Zihao Zang,Xiyuan Tao,Lingguang Yi,Xiaoyi Chen,Xiaoyan Zhang,Li Yang,Xianhu Liu,Xianyou Wang

All-solid-state lithium batteries (ASSLBs) composed of sulfide-based solid-state electrolyte and LiNixMnyCo1–x–yO2 (NMC) cathode are expected to become the promising next generation of energy storage systems due to their great potential in highly improved safety and energy density. However, the poor interfacial stability between the NMC cathode and sulfide-based electrolyte remains an important challenge for the commercialization of ASSLBs. In this study, a thin layer of fast lithium-ion conductor Li1.3Al0.3Ti1.7(PO4)3 (LATP) with a thickness of 8 nm was coated at the interface between LiNi0.8Co0.1Mn0.1O2 (NCM811) and Li5.5PS4.5Cl1.5 via a facile wet chemical method to improve interfacial stability. It has been found that the nanoscale LATP coating layer can not only accelerate lithium ions across the NCM811/Li5.5PS4.5Cl1.5 interface but also effectively alleviate the interfacial problems. The initial discharge capacity of the as-prepared LATP@NCM811/Li5.5PS4.5Cl1.5/Li batteries at 0.1 C is 151.5 mAh/g, and the capacity retention rate is 81.6% after 100 cycles at room temperature. The results indicate that interfacial modification with the nanosized LATP coating is an effective strategy for providing more possibilities for commercial application of ASSLBs.

研究领域: 材料科学 · 能源存储技术
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Ionic liquid-grafted MXene composite polymer electrolytes for high-performance solid-state batteries

Zhi Qian,Zhao-Dong Qiu,Rui-Qing Wang,Mei-Tong Wei,An-Min Fei,Zhi-Yi Hu,Hemdan S.H. Mohamed,Li-Hua Chen,Yu Li,Bao-Lian Su

All-solid-state batteries (ASSBs) have obtained much attention due to the high energy density and security. At present, PEO-based solid-state batteries are considered to be one of the most promising candidates for high-performance ASSBs due to the excellent processability and good interfacial stability. However, low ionic conductivity and Li + transference number seriously hinder their progress in practical applications. Here, a novel filler is developed by embedding ionic liquid (IL) grafted onto the surface of MXene to improve the electrochemical performance of PEO-based solid composite polymer electrolyte (MXene-IL-SPE) for ASSBs. The 2D MXene can significantly reduce the crystallinity of PEO, and the presence of IL not only enhances the dispersion of MXene in the polymer matrix, but also promotes the dissociation of lithium salts and anchors anions. As a result, the MXene-IL-SPE possesses high ionic conductivity (7.19 × 10 −4 S cm −1 ) and Li + transference number (0.51), together with wide electrochemical window (5.2 V) at 60 °C. The assembled LiFePO 4 |MXene-IL-SPE|Li full cell exhibits remarkable rate capability and exceptional capacity of 154.8 mAh g −1 over 120 cycles with an impressive 95.3 % capacity retention at 0.5 C. This design opens up a new way to prepare high performance CPEs for ASSBs.

研究领域: 材料科学 · 电化学
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ACS Nano · 2024 · IF 15.8

Superior Low-Temperature All-Solid-State Battery Enabled by High-Ionic-Conductivity and Low-Energy-Barrier Interface

Pushun Lu,Sheng Gong,Chuhong Wang,Zhiao Yu,Yuli Huang,Tenghuan Ma,Jingchen Lian,Zhiwen Jiang,Liquan Chen,Hong Li,Fan Wu

All-solid-state batteries (ASSBs) working at room and mild temperature have demonstrated inspiring performances over recent years. However, the kinetic attributes of the interface applicable to the subzero temperatures are still unidentified, restricting the low-temperature interface design and operation. Herein, a host of cathode interfaces are constructed and investigated to unlock the critical interface features required for cryogenic temperatures. The unstable interface between LiNi0.90Co0.05Mn0.05O2 (Ni90) and Li6PS5Cl (LPSC) sulfide solid electrolyte (SE) results in unfavorable cathode–electrolyte interphase (CEI) and sluggish lithium-ion transport across the CEI. After inserting a Li2ZrO3 (LZO) coating layer, the activation energy of the Ni90@LZO/sulfide SE interface can be reduced from 60.19 kJ mol–1 to 41.39 kJ mol–1 owing to the suppressed interfacial reactions. Through replacing the LPSC SE and LZO coating layer by the Li3InCl6 (LIC) halide SE, both a highly stable interface and low activation energy (25.79 kJ mol–1) can be achieved, thus realizing an improved capacity retention (26.9%) at −30 °C for the Ni90/LIC/LPSC/Li-In ASSB. Moreover, theoretical evaluation clarifies that cathode/SE interfaces with high ionic conductivity and low energy barrier are favorable to the Li+ conduction through the interphase and the Li+ transfer across the cathode/interphase interface. These critical understandings may provide guidance for low-temperature interface design in ASSBs.

研究领域: 材料科学 · 电化学
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ACS Nano · 2018 · IF 13.709

Core–Shell Fe1–xS@Na2.9PS3.95Se0.05 Nanorods for Room Temperature All-Solid-State Sodium Batteries with High Energy Density

Hongli Wan,Jean Pierre Mwizerwa,Xingguo Qi,Xin Liu,Xiaoxiong Xu,Hong Li,Yong-Sheng Hu,Xiayin Yao

High ionic conductivity electrolyte and intimate interfacial contact are crucial factors to realize high-performance all-solid-state sodium batteries. Na2.9PS3.95Se0.05 electrolyte with reduced particle size of 500 nm is first synthesized by a simple liquid-phase method and exhibits a high ionic conductivity of 1.21 × 10–4 S cm–1, which is comparable with that synthesized with a solid-state reaction. Meanwhile, a general interfacial architecture, that is, Na2.9PS3.95Se0.05 electrolyte uniformly anchored on Fe1–xS nanorods, is designed and successfully prepared by an in situ liquid-phase coating approach, forming core–shell structured Fe1–xS@Na2.9PS3.95Se0.05 nanorods and thus realizing an intimate contact interface. The Fe1–xS@Na2.9PS3.95Se0.05/Na2.9PS3.95Se0.05/Na all-solid-state sodium battery demonstrates high specific capacity and excellent rate capability at room temperature, showing reversible discharge capacities of 899.2, 795.5, 655.1, 437.9, and 300.4 mAh g–1 at current densities of 20, 50, 100, 150, and 200 mA g–1, respectively. The obtained all-solid-state sodium batteries show very high energy and power densities up to 910.6 Wh kg–1 and 201.6 W kg–1 based on the mass of Fe1–xS at current densities of 20 and 200 mA g–1, respectively. Moreover, the reaction mechanism of Fe1–xS is confirmed by means of ex situ X-ray diffraction techniques, showing that partially reversible reaction occurs in the Fe1–xS electrode after the second cycle, which gives the obtained all-solid-state sodium battery an exceptional cycling stability, exhibiting a high capacity of 494.3 mAh g–1 after cycling at 100 mA g–1 for 100 cycles. This contribution provides a strategy for designing high-performance room temperature all-solid-state sodium battery.

研究领域: 材料科学 · 能源存储与转换
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JOURNAL OF SOLID STATE CHEMISTRY · 2023 · IF 3.3

Enhanced electrochemical properties of Li2MgCl4 by Zn substitution for all-solid-state batteries

Zesen Gao,Shaowei Wang,Futing Sun,Zhiqian Yu,Hucheng Song,Zhanqiang Liu,Haijie Chen

Halides have currently been discovered to be ideal electrolytes for all-solid-state Li batteries (ASSLBs) due to their variability, splendid electrochemical stability, and high Li + conductivities. Here, we studied the electrochemical properties of Li 2-2 x Zn x MgCl 4 ( x  = 0–0.3) and their application in ASSLBs. By Zn substitution into the Li site of Li 2 MgCl 4 , the Li  +  conductivities of Li 1.6 Zn 0.2 MgCl 4 (1.2 × 10 −5  S/cm) at room temperature is two orders higher than that of Li 2 MgCl 4 (1.9 × 10 −7  S/cm). The activation energy is reduced to 0.28 eV for Li 1.6 Zn 0.2 MgCl 4 (Li 2 MgCl 4 is 0.47 eV). We attributed the enhanced electrochemical performance to Li vacancies generated from the Zn substitution. In addition, we fabricated a Li | Li 1.6 Zn 0.2 MgCl 4 | Li cell to appraise the electrochemical performance in the lithiation and stripping. It is demonstrated that Li 1.6 Zn 0.2 MgCl 4 can cycle for 100 h under a current density of 0.07 mA/cm 2 . This study demonstrates that introducing Li vacancy into Li 2 MgCl 4 may be a valid way to promote the electrochemical properties of the halides.

CAS / MDL: 7786-30-3
研究领域: 材料科学 · 电化学
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