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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-11 · IF 14.7

Entropy-increased LiMn2O4-based positive electrodes for fast-charging lithium metal batteries

Zeng Weihao,Xia Fanjie,Wang Juan,Yang Jinlong,Peng Haoyang,Shu Wei,Li Quan,Wang Hong,Wang Guan,Mu Shichun,Wu Jinsong

Fast-charging, non-aqueous lithium-based batteries are desired for practical applications. In this regard, LiMn 2 O 4 is considered an appealing positive electrode active material because of its favourable ionic diffusivity due to the presence of three-dimensional Li-ion diffusion channels. However, LiMn 2 O 4 exhibits inadequate rate capabilities and rapid structural degradation at high currents. To circumvent these issues, here we introduce quintuple low-valence cations to increase the entropy of LiMn 2 O 4 . As a result, the entropy-increased LiMn 2 O 4 -based material, i.e., LiMn 1.9 Cu 0.02 Mg 0.02 Fe 0.02 Zn 0.02 Ni 0.02 O 4 , when tested in non-aqueous lithium metal coin cell configuration, enable 1000 cell cycles at 1.48 A g −1 (corresponding to a cell charging time of 4 minutes) and 25°C with a discharge capacity retention of about 80%. We demonstrate that the increased entropy in LiMn 2 O 4 leads to an increase in the disordering of dopant cations and a contracted local structure, where the enlarged LiO 4 space and enhanced Mn-O covalency improve the Li-ion transport and stabilize the diffusion channels. We also prove that stress caused by cycling at a high cell state of charge is relieved through elastic deformation via a solid-solution transition, thus avoiding structural degradation upon prolonged cycling.

研究领域: 材料科学 · 电化学
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Materials · 2021 ·Vol. 14 ·期 12 ·3193 · IF 3.623

Preparation of LiFePO4 Powders by Ultrasonic Spray Drying Method and Their Memory Effect

Tu Lan,Xiaolong Guo,De Li,Yong Chen

The memory effect of lithium-ion batteries (LIBs) was first discovered in LiFePO4, but its origin and dependence are still not clear, which is essential for regulating the memory effect. In this paper, a home-made spray drying device was used to successfully synthesize LiFePO4with an average particle size of about 1 μm, and we studied the influence of spray drying temperature on the memory effect of LiFePO4in LIBs. The results showed that the increasing of spray drying temperature made the memory effect of LiFePO4strengthen from 1.3 mV to 2.9 mV, while the capacity decreased by approximately 6%. The XRD refinement and FTIR spectra indicate that the enhancement of memory effect can be attributed to the increment of Li–Fe dislocations. This work reveals the dependence of memory effect of LiFePO4on spray drying temperature, which will guide us to optimize the preparation process of electrode materials and improve the management system of LIBs.Keywords:LiFePO4;spray drying method;memory effect;cathode materials

研究领域: 材料科学 · 电化学
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Batteries-Basel · 2025 ·Vol. 11 ·期 4 ·142 · IF 4.8

Synthesis of Cathode Material Li2FeTiO4 for Lithium-Ion Batteries by Sol–Gel Method

Pengqing Hou,Qi Sun,Shengxue Yan,Guanglong Li,Yingdong Qu,Shaohua Luo

The development of a simple and reliable strategy to synthesize cathode materials is crucial for achieving the overall high performance of rechargeable lithium batteries, which has proved to be quite challenging. Herein, we report a simple sol–gel method for the synthesis of Li2FeTiO4cathode materials. The reaction mechanism of Li2FeTiO4crystals can be divided into five stages: including the breakage of the coordination bond; the thermal decomposition of citric acid; the thermal decomposition of metal salts and the reduction of trivalent iron and the formation of Li2FeTiO4crystals. Finally, the optimum calcination temperature for the preparation of Li2FeTiO4cathode materials was explored. The Li2FeTiO4cathode material prepared at 700 °C provides a discharge-specific capacity of 121.3 mAh/g in the first cycle and capacity retention of 89.2%. Our results provide new insights into the application of Li2FeTiO4cathode materials.

CAS / MDL: 6108-17-4 872-50-4
研究领域: 材料科学 · 电化学
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Energy Storage Materials · 2025 · IF 20.2

Direct regeneration of high-performance cathode materials from spent LCO batteries through in situ utilization of aluminum

Guisheng Zeng,Chongwen Hu,Rui Zhou,Juyong Wang,Xianfu Liu,Jianwen Huang,Jiaping Yu,Guanghui Wu,Zhongbing Wang,Chunjian Deng,Junwei He,Chunli Liu,Xubiao Luo

With the impending increase in the number of retired lithium-ion batteries, effective recycling and upcycling strategies must be explored to alleviate resource shortages, address environmental pollution, and meet the growing demand for high-performance cathode materials. This study proposes a closed-loop upcycling strategy that utilizes current collector aluminum (Al) as both a dopant and raw material for surface coating. This approach repairs the structural defects of highly degraded LiCoO 2 (LCO) cathode materials and achieves bulk Al doping and surface LiAlO 2 coating, transforming them into high-performance cathode materials capable of stable operation at a high voltage of 4.5 V. Specifically, bulk Al doping suppresses irreversible phase transitions and enhances structural stability, while the LiAlO 2 coating improves interfacial charge transfer and mitigates polarization. The synergistic effects of these modifications collectively enhance the electrochemical stability of LCO. The upcycled material delivers an initial discharge capacity exceeding 181.5 mAh g -1 and retains 93.9% of its capacity after 200 cycles at 1 C. Even under a high current rate of 10 C, the discharge capacity remains above 150.1 mAh g -1 , thereby outperforming commercial LCO cathodes. This study provides a simple and efficient solution for the direct upcycling of degraded LCO cathode materials into high-performance alternatives.

研究领域: 材料科学 · 环境科学
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Pollutant-free pyrolysis strategy for direct upgrading of cathode materials from spent lithium-ion batteries

Pengwei Li,Shaohua Luo,Guodong Hao,Kuo Sun,Qiuyue Liu,Martin Møller,Deyong Wang,Peter Kjær Kristensen,Leonid Gurevich,Lars Rosgaard Jensen,Li Wang,Xiangming He

The recycling of lithium-ion batteries (LIBs) has been dogged by air pollutants containing fluoride (e.g. HF, PF 5 , POF 3 ). Pyrolysis is a technique that can eliminate polyvinylidene fluoride (PVDF) from the cathode electrode sheets of spent LIBs, effectively separating the cathode material from the aluminum (Al) foil. Nonetheless, the HF gas generated during pyrolysis not only corrodes equipment but also presents serious environmental risks. To address this, a novel, eco-friendly strategy is introduced for the direct upgrading of cathode active materials (CAM). The strategy's cornerstone involves incorporating a minor amount of calcium into the original cathode material's coating, and it leverages mechanical stirring during the waste battery material separation process to ensure the electrode is fully detached from the current collector at a reduced temperature. The pyrolysis mechanism elucidates that fluorine-containing organic pollutants are converted into metal fluorides and deposited on the surface of cathode particles during aerobic pyrolysis, thereby improving the interfacial stability of lithium nickel cobalt manganese oxide (NCM) materials, reducing transition metal dissolution. This strategy not only eliminates the release of fluorine-containing organic pollutants during pyrolysis but also achieves direct regeneration of CAM. This work underscores the importance of the cathode materials' manufacturing process in facilitating the recycling of spent LIBs and provides an environmentally friendly and economically viable solution for the battery recycling industry.

研究领域: 环境科学 · 材料科学
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Nanoscale Research Letters · 2014 ·Vol. 9 ·期 1 ·1-5 · IF 2.481

Facile molten salt synthesis of Li2NiTiO4 cathode material for Li-ion batteries

Wang Yanming,Wang Yajing,Wang Fei

Well-crystallized Li 2 NiTiO 4 nanoparticles are rapidly synthesized by a molten salt method using a mixture of NaCl and KCl salts. X-ray diffraction pattern and scanning electron microscopic image show that Li 2 NiTiO 4 has a cubic rock salt structure with an average particle size of ca. 50 nm. Conductive carbon-coated Li 2 NiTiO 4 is obtained by a facile ball milling method. As a novel 4 V positive cathode material for Li-ion batteries, the Li 2 NiTiO 4 /C delivers high discharge capacities of 115 mAh g -1 at room temperature and 138 mAh g -1 and 50°C, along with a superior cyclability.

研究领域: 材料科学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2022 · IF 6.371

Environmental-friendly low-cost direct regeneration of cathode material from spent LiFePO4

Cai Qi,Shuhan Wang,Xukun Zhu,Tong Zhang,Yanju Gou,Zexin Xie,Yachao Jin,Yao Wang,Li Song,Mingdao Zhang

The green and low-cost recycling of spent LiFePO 4 (LFP) cathode materials has become an urgent problem to be solved. In this work, a completely green and easy scale-up recycling process is developed to recycle the cathode powders from spent LFP batteries. The optimal regeneration conditions are obtained by adjusting temperature, Li + concentration and reductant dosage. Meanwhile, the mechanism of regeneration is investigated by microscopic characterization and electrochemical performance testing. The regenerated LFP shows a good discharge specific capacity of 148 mAh/g at 0.05 C, which exhibits around 96% the capacity of raw LFP. Additionally, the costs of the consumption only account for 19.8% the price of raw LFP, which indicates that this method has good prospect of economic returns. This regeneration method is low in cost, simple in process, mild in conditions and easy to scale up, providing technical supports for the sustainable development of lithium-ion battery industry.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 环境科学
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International Journal of Electrochemical Science · 2023 · IF 1.5

Novel fabrication of Li4Ti5O12 coated LiMn2O4 nanorods as cathode materials with long-term cyclic stability at high ambient temperature

Chengyi Zhu,Jianxiong Liu,Xiaohua Yu,Yingjie Zhang,Xiaodong Jiang,Peng Dong,Yannan Zhang

Spinel LiMn2O4 has attracted increasing interest as promising cathode material owing to its low cost, high safety, and environmental friendliness. But the further development of LiMn2O4 is restricted by fast capacity fading upon cycling, especially at high temperatures. Herein, the one-dimensional (1D) Li4Ti5O12 coated LiMn2O4 nanorods (LMO-LTO) are successfully prepared by combining sol-gel and solid-state calcination method and ultimately enhance the cathode utilization in high-temperature and long-cycling conditions. The as-prepared LMO-LTO cathode delivers a high initial discharge capacity of 128.5 mAh g -1 at 0.1 C rate and exhibits a promising discharge capacity over 74.5 mAh g -1 at 10 C rate. Even under an elevated temperature of 55 O C, it still maintains 74.8% of its initial capacity at 1 C rate. Furthermore, the electrochemical impedance spectra (EIS) measurement confirm that compared with the pure LiMn2O4 nanorod, lower the charge transfer resistance (Rct) and enhanced Li + diffusion coefficient are also strong evidences of the improved electrochemical performance of LiMn2O4 nanorods after Li4Ti5O12 coating.

研究领域: 材料科学 · 电化学
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Nanomaterials · 2022 ·Vol. 12 ·期 5 ·886 · IF 5.719

Carbon Nanotube-Modified Nickel Hydroxide as Cathode Materials for High-Performance Li-S Batteries

Qianwen Jin,Yajing Yan,Chenchen Hu,Yongguang Zhang,Xi Wang,Chunyong Liang

The advantages of high energy density and low cost make lithium–sulfur batteries one of the most promising candidates for next-generation energy storage systems. However, the electrical insulativity of sulfur and the serious shuttle effect of lithium polysulfides (LiPSs) still impedes its further development. In this regard, a uniform hollow mesoporous Ni(OH)2@CNT microsphere was developed to address these issues. The SEM images show the Ni(OH)2delivers an average size of about 5 μm, which is composed of nanosheets. The designed Ni(OH)2@CNT contains transition metal cations and interlayer anions, featuring the unique 3D spheroidal flower structure, decent porosity, and large surface area, which is highly conducive to conversion systems and electrochemical energy storage. As a result, the as-fabricated Li-S battery delivers the reversible capacity of 652 mAh g−1after 400 cycles, demonstrating excellent capacity retention with a low average capacity loss of only 0.081% per cycle at 1 C. This work has shown that the Ni(OH)2@CNT sulfur host prepared by hydrothermal embraces delivers strong physical absorption as well as chemical affinity.Keywords:Li-S battery;carbon nanotube;nickel hydroxide;cathode

研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2024 · IF 5.4

High Entropy and Co-Free High Nickel Based Layered LiNi0.9Mn0.1O2 Cathode for Li-Ion Batteries

Seokyoung Choi,Wuliang Feng,Yongyao Xia

High nickel and Co-free layered cathodes (LiNi0.9Mn0.1O2, NM) for lithium-ion batteries (LIBs) have gained researchers’ interest recently because of their high energy density and being free of toxic elements, but they still suffer from inferior electrochemical performance due to the lattice instability during cycling. Herein, we successfully improved the electrochemical performance of NM using a high-entropy strategy. A high nickel Co-free multidoped high-entropy LiNi0.9Mn0.05Zr0.01Nb0.01Ti0.01Al0.01Mg0.01O2 (HE-NM, where HE represents high entropy with Zr, Nb, Ti, Al, and Mg dopants) cathode with five dopants was successfully synthesized. Owing to the effect of the multidopant, parasitic reactions and the accumulation of rock-salt phase were successfully suppressed, which led to uniformized interior stress and effectively inhibited microcracks during cycling. Consequently, HE-NM showed high thermal and structural stability with an initial discharge capacity of 206.35 mAh g–1 at 0.1 C and a retention of 76% after 100 cycles at 1 C, which showed a great advantage over the pristine NM (63%). This work provided a strategy for the stabilization of the NM cathode, which provided insight for the development of high-performance LIBs.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 能源存储
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Fluorinated carbonate-based electrolyte engineering solvation structure for high-voltage Li||LiNiO2 cell

Wei-Chen Zheng,Jin-Xia Lin,Hui Chen,Shi-Shi Liu,Chen-Guang Shi,Ling Huang,Shi-Gang Sun

Ni-rich layered oxides are considered ideal positive electrode materials for next-generation state-of-the-art Li-based batteries owing to their high energy densities. However, the structural degradation of Ni-rich positive electrodes and electrolyte decomposition presents significant challenges, particularly at high cut-off voltages. Herein, we report a novel electrolyte consisting of fluorinated solvents that enables the long lifespan of a Li||LiNiO 2 cell with a cut-off voltage of up to 4.5 V. The Li||LiNiO 2 cell retains 93.8% of its initial capacity after 200 cycles. The cycling stability was ascribed to the fluorinated solvents dominating the first structural shell of Li + and deriving a robust cathode-electrolyte interphase (CEI) on the positive electrode. Compared to commercial electrolytes, the fluorinated electrolyte inhibits the structural degradation, stress corrosion cracking, and interphase side reactions of the LiNiO 2 electrode. On the Li negative electrode side, ideal Li plating/stripping and the inhibition of the attack of Ni 2+ are achieved. Furthermore, the 4.5 V-Li||LiNiO 2 cell exhibited a capacity retention of 80.2% after 100 cycles, even under extremely fast-charging conditions.

研究领域: 材料科学 · 电化学
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Processes · 2025 ·Vol. 13 ·期 5 ·1525 · IF 2.8

Recycling Positive Electrode Materials of Li-Ion Batteries by Creating a pH Gradient Within Aqueous Sodium Chloride Electrolyser

Yue Chen,Xiaofei Guan

Recycling the positive electrode materials of spent Li-ion batteries is critical for environmental sustainability and resource security. To facilitate the attainment of the goal, this study presents a novel approach for recovering valuable metals from positive electrode materials of spent lithium-ion batteries (LIBs) in an H-shaped cell containing aqueous NaCl electrolyte. The process employs hydrochloric acid that could be derived from the chlorine cycle as the leaching agent. The electrolytic device is engineered to generate a high pH gradient, thereby enhancing the leaching of metal elements and eliminating the requirement for external acid or base addition. This green recycling approach adheres to the principles of a circular economy and provides an environmentally friendly solution for sustainable battery material recycling.

CAS / MDL: 7647-14-5
研究领域: 环境科学 · 材料科学
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