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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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Science China-Chemistry · 2025 · IF 9.7

Controllably elevating the initial Coulombic efficiency of Li3VO4 anode via a facile electrode pre-lithiation technique for lithium-ion batteries

Liang Haoyue,Zhong Xingguo,Huang Guxin,Liu Wenpan,Liu Yao,Wang Shuhao,Wang Deyu,Liu Hao,Wang Hao,Zhai Tianyou,Li Huiqiao

Li 3 VO 4 has been a promising insertion anode material for Li-ion batteries, which has high theoretical capacity (up to ∼600 mAh g −1 ) and safe Li insertion voltage (0.5–1 V vs. Li/Li + ). However, the low initial Coulombic efficiency (ICE) has always been the bottleneck limiting its commercialisation. Here, we propose a facile pre-lithiation method to controllably elevate the ICE by the post-treatment of the prepared Li 3 VO 4 composite electrode based on an immersion reaction. In this process, the whole electrode was immersed in the liquid Li source, via which the ICE of the Li 3 VO 4 electrode can be controllably elevated from 80% to over 100% within 5 min of pre-lithiation. Rather than the traditional powder treatment for pre-lithiation, this process we proposed minimizes the impact of pre-lithiation on the battery assembly process. Moreover, we further investigated the effect of this pre-lithiation process on the functional components in the electrode. For the first time the ICE of Li 3 VO 4 electrode was elevated to 100%. As a result, the initial reversible capacity of LiFePO 4 ∥Li 3 VO 4 full cell was improved from 44.0 to 146.3 mAh g −1 , demonstrating the feasibility and great potential of the process.

CAS / MDL: 9004-32-4 9085-26-1
研究领域: 材料科学 · 电化学 · 能源存储
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ChemSusChem · 2025 · IF 6.6

PF6- and Na+ Co-intercalation in Graphite Cathode of Sodium Dual-Ion Batteries by Enhanced Surface Concentration Effect

Fan Li,Yong-Feng Shen,Bin He,Wen-Cui Li

Dual-ion batteries are attracting much attention due to the joint participation of anions and cations in the energy storage process. However, this unique battery configuration imposes high demands on the cathode, which typically presents an inferior rate performance. Herein, we employ graphite in different microcrystalline sizes as cathodes, associated with high concentration electrolyte to construct sodium dual-ion batteries. The results of in-situ XRD and Raman evidence that the surface effect is enhanced by suitably small graphite microcrystals, where a greater surface involvement affords more electro-activated regions for the ions. Furthermore, the analysis of sputtering XPS confirms that the PF6- is accompanied by the co-intercalation of Na+ into cathodes by constructing the model of concentration effect, thus accelerating the kinetic process. In conclusion, the co-intercalation of PF6- together with Na+ is demonstrated under the influence of enhanced surface concentration effect in cathodes, and thus the cathodes exhibit a superior rate performance with a capacity of 103.6 mAh g-1 at a rate of 2 C and a rate retention of 94.8% even at 50 C. This work provides new insights to explain the mechanism of ion intercalation in dual-ion batteries and offers a perspective for the construction of high energy storage systems.

CAS / MDL: 7782-42-5
研究领域: 材料科学 · 电化学
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SOLID STATE IONICS · 2024 · IF 3

Sulfur-doped porous carbon derived by metal-organic framework (MOF-5) for high lithium/sodium storage performance

Qin Zhou,Cong Xia,Ji Li,Amei Cheng,Jianwen Liu,Hongying Liu,Lin Li,Shiquan Wang

Metal-organic framework (MOF-5) material was synthesized by solvothermal method. Porous carbon (C) and sulfur-doped porous carbon (S/C) were fabricated by calcining and vulcanization of MOF-5. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and Raman spectroscopy were used to characterize the crystal structure and morphology of the samples. The electrochemical performance of C and S/C materials were tested as anode materials for lithium ion batteries (LIBs) and sodium ion batteries (SIBs). The S/C exhibits the high reversible capacity (1114.8 mAh g −1 after 100 cycles at 0.1 A g −1 and 485 mAh g −1 after 500 cycles at 2.0 A g −1 ), as anode for LIBs. It behaves a reversible discharge capacity of 268.8 mAh g −1 after 100 cycles at 0.1 A g −1 and a capacity of 157 mAh g −1 after 1000 cycles at 2.0 A g −1 , as anode for SIBs. Compared with C, the electrochamical performance of S/C material is significantly improved. This is mainly because the bigger specific surface area and the doping of sulfur atoms increases the layer spacing and facilitates the kinetics of the intercalation and deintercalation of Li + and Na + ions, especially Na + ions.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

Ionic liquid additive stabilized cathode/electrolyte interface in LiCoO2 based solid-state lithium metal batteries

Qipeng Zhang,Kecheng Pan,Mengmin Jia,Xiaoyan Zhang,Lan Zhang,Haitao Zhang,Suojiang Zhang

Poly(ethylene oxide) (PEO)-based solid state batteries is one of the most attractive candidates for next-generation high performance energy storage devices, especially when it matches the LiCoO 2 cathode of high volumetric energy density. However, cathode/electrolyte interface reactions will be triggered at high voltage, leading to high interfacial resistance and fast capacity decay. In this work, a selected ionic liquid , 1-methyl-1-propylpiperidinium tetrafluoroborate (PP 13 BF 4 ), is prepared and applied in LiCoO 2 electrode operating at high work voltages of 3.0–4.3 V to regulate the interface. Electrochemical impedance spectroscopy and holding test indicate that facilitated by the PP 13 BF 4 , the cathode/electrolyte interfacial reaction is effectively suppressed and the resistance is reduced. When an optimal content, 2  wt%, PP 13 BF 4 is added into the LiCoO 2 electrode, the solid-state lithium metal cell delivers an initial discharge capacity of 125.1 mAh g −1 under the current density of 0.05 C at 55 °C, which is almost twice that of bare electrode. Meantime, it retains 76.3% of its capacity in 100 cycles under 0.2 C rate. Further characterizations illustrate that PP 13 BF 4 participates in the formation of a protective CEI, which effectively suppresses parasitic reactions between electrolyte and electrode. This work provides a facile and practical idea for the development of 4 V class solid state lithium metal batteries .

CAS / MDL: 626-67-5 106-94-5
研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2013 ·Vol. 1 ·期 47 ·15016-15021 · IF 0

Improvement in LiFePO4–Li battery performance via poly(perfluoroalkylsulfonyl)imide (PFSI) based ionene composite binder

Qianru Shi,Lixin Xue,Zengbin Wei,Fu Liu,Xudong Du,Darryl D. DesMarteau

Lithiated poly(perfluoroalkylsulfonyl)imide (PFSILi) ionene is synthesized and blended with poly(vinylidene) difluoride (PVDF) to serve as binder for the electrode of a lithium ion battery. The incorporation of the PFSILi ionene adds ionic conducting channels inside the electrodes and prevents electrolyte depletion during rapid charging–discharging. The small composition change results in an increase in the battery performance, including a better reversibility, lower polarization or internal resistance and an improved discharge capacity, as well as a higher energy density at high rates or elevated temperatures. At the rate of 2 C and 60 °C, the discharge plateau potential for the cell with the ionene based binder is 0.29 V higher than that for the cell with a PVDF only cathode binder. At a 4 C rate, the discharge capacity and energy density of a LiFePO4–Li half-cell with the ionic binder are 50% and 66%, respectively, higher than those of the cell using the nonionic PVDF binder at room temperature. Thus, the ionene polymer offers a new route, rather than just altering the active materials, to overcome the limitations of capacity and power density for rechargeable lithium batteries.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 电化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2024 · IF 4.1

Online cell pressure tracking analysis and sulfur species depositing/stripping behavior study of lithium sulfur batteries

Chuanxin Zong,Bo Hong,Furong Qin

Cell failure is easy occurring in Li-S cell. Electrolyte consumption caused by side-reactions between electrolyte and anode is one of the reasons for the cell failure, but the underlying mechanism for the cell failure is still not clear. To get insight into the electrolyte decomposition, in this work, online cell pressure tracking analysis (OCPTA) is applied to study the gassing effect caused by electrolyte decomposition reactions during charge–discharge processes and the study on depositing/stripping behavior of sulfur species performed. It is found that gassing effect is negligible in the cell with conventional ether-based electrolyte when electrolyte decomposing, but volume effect caused by sulfur species dissolution is notable. Together with the sulfur preferentially depositing on the top surface of cathode, it leads to electrolyte insufficiency on the top surface of electrodes, enhancing the risk of cell failure.

CAS / MDL: 67-68-5
研究领域: 材料科学 · 电化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY · 2023 · IF 4.5

Exploring the effect of lithium halide artificial SEI on the electrochemical performance of lithium metal batteries

Xintai Xie,Jinbiao Chen,Xuanyi Chen,Zhicong Shi

The urgent need for high-energy–density rechargeable batteries is driving lithium (Li) metal as a promising anode material. However, the conventional solid electrolyte interface (SEI) on lithium metal suffers from elevated interfacial impedance, poor mechanical properties, and non-uniform Li + flux. Previously, LiF has been proven to be an effective component of the SEI protecting lithium metal. However, this is a rarely reported application of LiCl and LiBr in SEI. Herein, we design SEI containing lithium halide in different ratios (LiF 0.8 Cl 0.1 Br 0.1 , LiF 0.33 Cl 0.33 Br 0.33 , LiCl, LiBr) to investigate the action laws of lithium halide in SEI. It has been shown that the performance of SEI containing lithium halide against lithium anode increases with the LiF content in the SEI. The higher the proportion of LiF in SEI, the better the cycle life and stability of Li-Li symmetric cells, and the higher the initial capacity and the capacity retention of LFP-Li full cells. The symmetric cell with LiF 0.8 Cl 0.1 Br 0.1 @Li has the smallest average polarization voltage (about ± 30 mV) and long cycle life of up to 1000 h. LiFePO 4 ||LiF 0.8 Cl 0.1 Br 0.1 @Li cells have the highest initial capacity (127.4 mAh/g), and still had 83.6 % capacity retention after 1000 cycles at 2C.

CAS / MDL: 872-50-4 109-99-9
研究领域: 材料科学 · 电化学 · 储能技术
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Nature Energy · 2025 · IF 60.1

Self-adaptive electrolytes for fast-charging batteries

Zhao Chang-Xin,Li Zheng,Chen Bin,Chen Fu,Wang Chunsheng

Fast charging of high-energy batteries is critical for transportation electrification but remains challenging because the rapid rise in cell overpotential easily exceeds electrolytes’ fixed electrochemical stability window. Here we design a self-adaptive electrolyte with a dynamically expanding electrochemical stability window that increases in real time during charging, outpacing the rise in overpotential as the charging current intensifies. The self-adaptive electrolyte is a single-phase solution of salt and complementary oxidation- and reduction-resistant solvents at the cloud point composition but can undergo solvent separation to dynamically redistribute solvent components during charging. The oxidation-resistant solvents concentrate at the positive electrode and reduction-resistant solvents accumulate at the negative electrode, broadening the electrolyte stability window in real time during charging. Proof-of-concept experiments validate the versatility of this design in both aqueous zinc-metal and non-aqueous lithium-metal batteries, achieving high Coulombic efficiencies of negative electrodes and enhanced oxidative stability for positive electrodes.

研究领域: 储能技术 · 电化学 · 电池技术 · 材料科学 · 交通电气化
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JOURNAL OF POWER SOURCES · 2021 · IF 9.127

Multidimensional VO2 nanotubes/Ti3C2 MXene composite for efficient electrochemical lithium/sodium-ion storage

Hao Liu,Pan He,Jiaxin Cao,Tao Duan,Qingquan Kong,Weitang Yao

The nature of vanadium oxides with multiple valence states and a rich species of oxides facilitates the construction of high performance batteries. Among these, vanadium dioxide (VO 2 ), despite offering several advantages, is seldom reported in anode materials due to its inferior cycling stability and rate performance caused by large volume changes. Herein, we employed a rational structural strategy to assemble VO 2 -NTs/Ti 3 C 2 anode with a multidimensional cross-linked structure using VO 2 nanotubes (VO 2 -NTs) and Ti 3 C 2 T x MXene . Specifically, the abundant multidimensional channels of VO 2 -NTs/Ti 3 C 2 reduce the diffusion impedance of the ions, and the enhanced intrinsic conductivity and highly robust structure solve the problems originally present in VO 2 , which are verified in characterization and density functional theory calculations. Consequently, the composite electrode shows ultra-high reversible capacity (1425 mAh g −1  at 1 A g −1 ), excellent cycling performance (516 mAh g −1  at 5 A g −1 after 2000 cycles) and superior rate performance (703 mAh g −1  at 10 A g −1 ), and also exhibits decent sodium storage performance, representing the best comprehensive battery performance of VO 2 -based anodes to date.

研究领域: 材料科学 · 电化学 · 储能技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Recycling cobalt from spent lithium-ion batteries for designing the novel cobalt nitride followers: Towards efficient overall water splitting and advanced zinc-air batteries

Zhuang Wang,Mian Li,Bin Fu,Wenping Cao,Xiangjie Bo

Although cobalt nitride (CoN)-based nanomaterials have been widely designed as advanced oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and oxygen reduction reaction (ORR) catalysts, the continuous consumption of lithium-ion batteries (LIBs) has led to a high price of cobalt metal. Therefore, in the future, recycling valuable Co elements from spent devices and boosting their service efficiency will inevitably promote the utilization of Co-based materials in water splitting and zinc-air batteries (ZABs). Herein, we realize the Co recycling from spent LIBs by a simple hydrometallurgy method. Under the assistance of hexamethylenetetramine and polystyrene spheres, after the hydrothermal and pyrolysis treatment in the NH 3 atmosphere, the as-reclaimed cobalt oxalates were successfully transformed into novel three-dimensional (3D) CoN nanoflowers (denoted as CoN NFs). Benefiting from the unique 3D flower-like architectures, intrinsic high conductivity, large surface area, uniformly dispersed CoN nanoparticles, and the synergistic effect between Co 3 N and CoO phases, the 3D flower-like CoN NFs exhibited excellent OER catalytic activity. The performance was much better than commercial RuO 2 in the 1.0 M KOH solution. Furthermore, the CoN NFs-based water splitting cell needed a voltage of 1.608 V to achieve the current density of 10 mA cm −2 , which is even 16 mV smaller than that of Pt/C||RuO 2 benchmark (1.624 V). Meanwhile, the CoN NFs-derived ZAB exhibited a high peak power density of 107.3 mW cm −2 (vs. 103.2 mW cm −2 of Pt/C-RuO 2 -based ZAB) and a low charge–discharge voltage gap (0.93 V vs. 1.43 V of Pt/C-RuO 2 -based ZAB). Due to the excellent structural and elemental stabilities, the corresponding water splitting cell and ZAB had outstanding durability. This work successfully explored an advanced industrial chain from recycling Co metal in spent devices to designing the high-efficiency HER/OER/ORR electrocatalysts for advanced water splitting devices and ZABs. This will further promote the value-added utilization of valuable Co metal in various energy storage or conversion devices.

研究领域: 材料科学 · 能源技术
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

LaCoO3 doping in PVDF-based electrolytes with long-cycle performance and excellent interface compatibility of solid-state batteries in a wide temperature range

Yan He,Jinpeng Guo,Chuanchuan Bi,Zhifei Hao,Bin Zhao,Chunping Li,Xiaogang Han,Qi Wang

Composite polymer electrolytes (CPE) have attracted considerable attention due to their potential to achieve high flexibility and large energy density. However, their practical application is hampered by their suitability at a single temperature and severe lithium dendrite growth. In this work, we have doped the perovskite inorganic filler LaCoO 3 into polyamide (PI) nanofibers and constructed a LaCoO 3 /PI/PVDF CPE. Electrochemical characterization of the CPE and density functional theory calculations performed for it show that perovskite nanofibers have abundant oxygen vacancies, which are conducive to accelerating the dissociation of lithium salts and releasing more free lithium ions. Li//Li symmetric batteries exhibit excellent long cycle performance (over 3000 h) at 30 °C, and LiFePO 4 //Li batteries exhibit excellent cycling performance with over 1000 cycles at (0.5 C, 30 °C) and 400 cycles at (0.2 C, 60 °C), which can be realized with high voltage cathode NMC 811. The physical properties of the CPEs are also quite outstanding, with good thermal stability as it can withstand a high temperature of 200 °C and tensile strength up to 12.01 MPa. This work presents a new idea for designing CPEs with high safety and excellent electrochemical properties, which can provide stable circulation over a wide temperature range.

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 电化学
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