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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

Li1.5Al0.5Ge1.5(PO4)3 membrane electrodialysis for lithium enrichment

Zhouyang Jiang,Wenhan Kong,Fenglin Zhao,Qingyue Han,Yangxi Liu,Suqing Wang,Haihui Wang

Highly purified LiOH is a common raw material of cathode active materials of lithium-ion batteries. Its demand is rapidly increasing with the fast development of the electric vehicles. The traditional enrichment process of LiOH relying on water evaporation requires a lot of energy. Here, we demonstrate the ability of NASICON-type Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 membrane electrodialysis to enrich the LiOH aqueous solution with a low concentration. This Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 membrane electrodialysis could extract 99.7% and 96.5% of Li + in 0.1, and 0.01 M LiOH feed solution, respectively, into 1 M LiOH receiving solution. And the transmembrane resistance between feed solution and receiving solution increased by 37.4, 389.5, and 964.6 Ω cm 2 , compared to the value for 1 M of LiOH feed solution as the feed solution concentration decreased to 0.1, 0.01 and 0.001 M, respectively. This quantitative assessment method for the resistance variation is crucial to the potential separation application of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 membrane electrodialysis in salt-lake brine.

研究领域: 材料科学 · 能源工程
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JOURNAL OF MEMBRANE SCIENCE · 2024 · IF 8.4

Enhanced Mg2+/Li+ separation by amino crown ether composite nanofiltration membrane with Mg2+ transport barrier

Yingyao He,Guiliang Li,Haibo Lin,Qiu Han,Yinlu Ye,Jianqiang Wang,Fu Liu

Selective separation property enhancement is quite important for membranes separations, especially for high mass ratio Mg 2+ /Li + separations. Low selectivity and unclear separation mechanism are the challenges for current membranes. In this study, we designed 4-aminophenyl-15-crown-5 incorporated polyamide nanofiltration membranes through interfacial polymerization for Li + enrichment. The electrochemical tests and energy barrier calculations using transition state theory confirmed that the crown ether in nanofiltration membrane is responsible for governing Mg 2+ transportation, resulting in a substantial energy barrier impeding its transport. Furthermore, a two-stage nanofiltration process was employed to enhance Li + enrichment in simulated brine and achieved 35-fold increase in Li + enrichment using as-fabricated membranes. These results demonstrate the substantial potential for Li  +  extraction from brine with a high Mg 2+ /Li + mass ratio using the crown ether incorporated membrane. Meanwhile, the proposed strategy incorporating transport barriers presents a novel approach for designing ion-selective channels within membranes.

研究领域: 材料科学 · 环境工程
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ELECTROCHIMICA ACTA · 2025 · IF 5.6

FePO4-Zn/Pt hybrid battery system for the electrochemical extraction of Li+ from salt lake brine with high Mg2+ concentrations

Qian Zhang,Xinwen Li,Kang Chen,Ying Hu,Rongmei Liu,Guixiang Qian,Zhongliang Tian,Chao Yang

This study presents a FePO 4 -Zn/Pt hybrid power battery system designed for lithium extraction from salt lake brines. Initially, the FePO 4 -Zn battery is utilized for lithium intercalation to form LiFePO 4 , which is subsequently reassembled into a LiFePO 4 -Pt battery for lithium deintercalation. As a result, a Li + -rich aqueous solution, free from interfering metal cations, is obtained. The system eliminates the need for ion-exchange membranes, as the Pt electrode remains separated from the brine, thereby preventing contamination by impurity cations. When applied to a brine containing 0.25 g/L Li + and 73 g/L Mg 2+ , followed by desorption in a solution of 0.25 g/L Li + , only a minimal amount of Mg 2+ was transferred to the lithium chloride solution after two cycles, achieving effective lithium extraction and enrichment with an efficiency of 80.6%.

研究领域: 电化学 · 能源材料 · 环境工程 · 分离科学 · 无机化学 · 资源循环利用
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Energy & Environmental Science · 2022 ·Vol. 15 ·期 8 ·3470-3482 · IF 39.714

Highly reversible Li2RuO3 cathodes in sulfide-based all solid-state lithium batteries

Yuqi Wu,Ke Zhou,Fucheng Ren,Yang Ha,Ziteng Liang,Xuefan Zheng,Zhenyu Wang,Wu Yang,Maojie Zhang,Mingzeng Luo,Corsin Battaglia,Wanli Yang,Lingyun Zhu,Zhengliang Gong,Yong Yang

The practical application of high-capacity lithium-rich cathode materials in lithium-ion batteries has been largely restricted by severe side reactions with electrolytes. Herein, we report a highly stable lithium-rich Li2RuO3 cathode by forming a passivating solid electrolyte interphase at the interface with a sulfide solid electrolyte such as Li6PS5Cl in all-solid-state lithium batteries (ASSLBs), which efficiently suppresses serious parasitic interfacial reactions and fast-increasing interfacial impedance normally observed in liquid electrolytes. The exceptionally high interfacial stability of the Li2RuO3/sulfide electrolyte interface contributes to a high reversible capacity of 257 mA h g−1 of Li2RuO3 at 0.05C rate, and unprecedented cycling stability with 90% capacity retention after 1000 cycles at 1C rate. Comprehensive experimental characterizations and first-principles calculations disclose that electronically insulating interfacial reaction products forming at the interface between the Li2RuO3 cathode and Li6PS5Cl facilitate the formation of a stable and passivating interphase and block the continuous side reactions. Importantly, reversible oxygen redox activity of Li2RuO3 is well-maintained in this configuration of ASSLBs even after 600 cycles, thus the common voltage decay of the Li-rich material is also significantly reduced. These new discoveries demonstrate the critical role of interface design for achieving prolonged cycling stability of lithium-rich cathode materials.

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

Highly miscible phases in lithium rich manganese-based cathode materials through simple heat treatment control

Zhaojin Li,Jialin Ren,Yifei Wang,Di Zhang,Qiujun Wang,Qujiang Sun,Ranran Li,Fei Yuan,Yufeng Zhu,Bo Wang

Li-rich Mn-based materials composed of C 2/ m and R -3  m mixed phases are considered to be the most promising cathode materials for lithium-ion batteries because of their extremely high specific capacity. However, these materials suffer from serious problems such as metal element leaching, oxygen release, and capacity decay during the cycling process. Realizing high mixing of two phases at the atomic level is an important measure to improve material stability, but there is a lack of methodological guidance. Here, we reported that adopting segmented calcination during the pre-calcination can regulate the forms and concentration of defects, the ratio of C 2/ m phase to R -3  m phase, and the grain size in the materials, thereby achieving effective control over the phase solubility and structural stability in the Li-rich Mn-based materials. With the same pre-calcination time, the sample that pre-sintered for 4 h in the first stage and 1 h in the second stage exhibited the best miscibility, thereby demonstrating excellent electrochemical performance, with a high reversible specific capacity of 230 mAh·g −1 at 0.1C and an incredible capacity retention of 87.7 % after 500 cycles.

研究领域: 材料科学 · 电化学 · 固态化学
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ELECTROCHIMICA ACTA · 2023 · IF 6.6

High-voltage all-solid-state lithium batteries with Li3InCl6 electrolyte and LiNbO3 coated lithium-rich manganese oxide cathode

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 · 电化学 · 能源存储 · 固态离子学 · 先进电池技术
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Nanomaterials · 2025 ·Vol. 15 ·期 13 · IF 4.3

Enhancing the Performance of LLO Through Vanadium Doping and Abundant Exposed (010) Planes in Secondary Particles

Shenghua Yuan,Chengwen Ren,Ziwei Liu,Yu Chen,Wenhui Wang

Lithium-rich layered oxide (LLO) has received extensive attention from researchers due to its high initial discharge capacity (≥250 mAh g−1). However, defects such as its high initial irreversible capacity, voltage decay, and poor rate performance have severely limited its commercialization. These issues arise because the Li2MnO3component in LLO is activated during the initial cycle, leading to the participation of lattice oxygen anions (O2−) in redox reactions. This results in irreversible oxygen loss (O2) and subsequent structural phase transitions. To address these challenges, this study focuses on Li1.2Ni0.13Co0.13Mn0.54O2as the host material, utilizing abundant exposed (010) plane secondary particles and employing a vanadium (V) doping strategy to enhance electrochemical performance. The V forms strong V-O bonds with the lattice oxygen, effectively suppressing irreversible oxygen loss and improving structural stability. The results demonstrate that the LLO achieves the best electrochemical performance as the doping amount is 1 mol%, and the capacity retention improves from 74.5% (undoped) to 86% (V-doped) after 140 cycles at 0.5 C.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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ACS Applied Engineering Materials · 2024 · IF 0

Fluorine-Doped Electrolyte and Artificial SEI for Enhanced Interfacial Stability in All-Solid-State Lithium Metal Batteries

Linfeng Peng,Tianyu Lei,Cong Liao,Shuai Chen,Shijie Cheng,Jia Xie

The poor lithium metal/solid electrolyte (SE) interface compatibility presents a considerable obstacle in the progression of all-solid-state lithium metal batteries (ASSLMBs). Constructing a robust solid electrolyte interphase (SEI) offers a favorable approach to alleviating these difficulties. Herein, we propose a dual strategy involving fluorine-doped electrolyte and artificial SEI to improve the lithium metal/Li5.5PS4.5Cl1.5 (LPSC) interface stability. X-ray photoelectron spectroscopy (XPS) results unveil the formation of a LiF-rich interphase at the SE/Li metal interface, facilitated by the reaction of Li metal with an F-doped electrolyte and fluoroethylene carbonate (FEC) treatment on the Li metal surface (FEC@Li). The F-doped electrolyte Li5.5PS4.5Cl1.45F0.05 (LPSCF-0.05) maintains a high ionic conductivity of 6.37 mS cm–1 at room temperature. Consequently, the critical current density (CCD) of the Li metal symmetric cell reaches 3.52 mA cm–2. Full cells assembled with NCM622, LPSCF-0.05, and FEC@Li exhibit superior cycling and rate performances along with excellent low-temperature performance. The battery delivers a high initial discharge capacity of 172.6 mAh g–1 at 0.2C under room temperature, cycling steadily for over 100 cycles. Under a high C-rate of 2C and a low temperature of −20 °C, the batteries display high capacities of 117.7 and 139.0 mAh g–1, respectively. This study offers an effective way of constructing high-performance ASSLMBs.

研究领域: 材料科学 · 电化学 · 能源存储 · 固态离子学 · 电池技术
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Lithium-Rich Solid Polymer Electrolytes Enabled by Thermal-Assisted Dual-Phase Dissociation for Highly Stable Flexible Electrochromic Devices

Bingqiang Ding,Qingchao Fan,Xilu Wu,Yingying Hao,Bingwei Bao,Qinghong Zhang,Yaogang Li,Chengyi Hou,Kerui Li,Hongzhi Wang

Flexible electrochromic (EC) devices with controllable optical modulation can adapt to irregular curved surfaces, offering great potential for wearable technologies and energy-saving applications. However, for solid polymer electrolytes (SPEs) that serve as a critical component in the EC devices, challenges remain in addressing the tradeoff between their ionic conductivity and mechanical strength. Herein, a lithium-rich solid electrolyte (LiRSE) is developed via a dual-phase dissociation of excess LiBF 4 , involving a liquid-phase deep eutectic solvent (DES) and a solid-phase polyurethane polar matrix. Assisted by the thermal pressing, the DES promotes the dissociation of excess Li salt and the activation of the previously inactive crystalline regions of polyurethane to release abundant polar groups for complexation with the excess Li salt. Thus, the LiRSE shows excellent ionic conductivity of 1.14 × 10 −4 S cm −1 , which is about 3.7 times higher than the electrolyte without dual-phase dissociation of excess LiBF 4 (3.07 × 10 −5 S cm −1 ). At last, a large-area LiRSE film with high transmittance of 88.7% and interfacial adhesion of 0.54 MPa is fabricated to assemble flexible EC devices with a fast switching speed (2.5 s/4.5 s), long cycling stability (94.1% after 7500 cycles), and wide-temperature stability.

CAS / MDL: 14283-07-9
研究领域: 材料科学 · 电化学 · 高分子科学 · 纳米技术 · 储能技术
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Frontiers in Chemistry · 2021 · IF 5.221

Li-Rich Antiperovskite/Nitrile Butadiene Rubber Composite Electrolyte for Sheet-Type Solid-State Lithium Metal Battery

Bian Juncao,Yuan Huimin,Li Muqing,Ling Sifan,Deng Bei,Luo Wen,Chen Xuedan,Yin Lihong,Li Shuai,Kong Long,Zhao Ruo,Lin Haibin,Xia Wei,Zhao Yusheng,Lu Zhouguang

Lithium-rich antiperovskites (LiRAPs) hold great promise to be the choice of solid-state electrolytes (SSEs) owing to their high ionic conductivity, low activation energy, and low cost. However, processing sheet-type solid-state Li metal batteries (SSLiB) with LiRAPs remains challenging due to the lack of robust techniques for battery processing. Herein, we propose a scalable slurry-based procedure to prepare a flexible composite electrolyte (CPE), in which LiRAP (e.g., Li2OHCl0.5Br0.5, LOCB) and nitrile butadiene rubber (NBR) serve as an active filler and as a polymer scaffold, respectively. The low-polar solvent helps to stabilize the LiRAP phase during slurry processing. It is found that the addition of LOCB into the NBR polymer enhances the Li ion conductivity for 2.3 times at 60°C and reduces the activation energy (max. 0.07 eV). The as-prepared LOCB/NBR CPE film exhibits an improved critical current of 0.4 mA cm−2 and can stably cycle for over 1000 h at 0.04 mA cm−2 under 60°C. In the SSLiB with the sheet-type configuration of LiFePO4(LFP)||LOCB/NBR CPE||Li, LFP exhibits a capacity of 137 mAh/g under 60 at 0.1°C. This work delivers an effective strategy for fabrication of LiRAP-based CPE film, advancing the LiRAP-family SSEs toward practical applications.

研究领域: 材料科学 · 电化学 · 电池技术
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