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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Enhanced Rapid and Efficient Recycling of Lithium-Ion Battery Cathode by Synergistic Effects of Ternary Deep Eutectic Solvents ChCl/MClx/Levulinic Acid

Fengyi Zhou,Yurun Tian,Hongyuan Zhang,Yijun Yin,Zeyu Wang,Rui Qin,Yu Chen,Zhiyong Li,Tiancheng Mu

The rapid growth of spent lithium-ion batteries (LIBs) raises concerns over the supply chain of critical metals and environmental impacts, emphasizing the urgent need for efficient recycling technologies. Due to their potential to reduce the consumption of energy and avoid the use of corrosive acid, deep eutectic solvents (DESs) have been widely studied to selectively leach and recover valuable metals from spent LIBs. There is general agreement that DESs with high acidity, coordination, reducibility, and low viscosity could efficiently dissolve cathode materials. However, it is hard to design binary DES compositions to fulfill all of these requirements simultaneously. Herein, this study focuses on the design of ternary DESs, leveraging the synergistic effects of their components to achieve strong coordination and low viscosity, enhanced acidity, and reducibility to efficiently extract valuable metals. Specifically, ChCl/CuCl:4Levulinic acid demonstrated exceptional leaching capabilities, recovering over 90% of LiCoO2 within 10 min. Furthermore, to ensure the purity of recovered metal products, ChCl/LiCl:8Levulinic acid was investigated to realize the efficient leaching, recovery, and DES regeneration process. It was verified that ChCl/LiCl/8Levulinic acid has high leaching efficiency and good cycling stability and facilitates a convenient recycling process. Overall, this work demonstrates the potential of tailored ternary DESs for the efficient leaching of cathode materials and proposes a sustainable process to realize metal recovery from spent LIB cathode and DES regeneration.

CAS / MDL: 7791-13-1
研究领域: 材料科学 · 环境科学 · 化学工程
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

A superior sodium-ion battery based on tubular Prussian blue cathode and its derived phosphide anode

Mingwei Jiang,Lingbo Ren,Zhidong Hou,Wei Hua,Da Lei,Yunjing Cao,Yu Zhang,Jian-Gan Wang

Sodium-ion batteries are receiving incremental attention as a promising alternative of the commercial lithium-ion batteries. However, it remains a challenging task to fully explore suitable cathode and anode materials for assembling a full cell with attractive Na-ion storage properties. Herein, we demonstrate a superior sodium-ion battery by pairing a tubular Prussian blue (PB) cathode and its derived phosphide anode. The tubular configuration endows the PB with fast reaction kinetics and thus delivers a large specific capacity of 94.4 mAh g −1 even at a high rate of 5.0 A g −1 . The PB-derived phosphide is featured by encapsulation of FeP nanoparticles into a conductive carbon matrix, which enables remarkable sodium energy storage likewise. Impressively, the as-assembled sodium-ion full cell exhibits an unprecedented capacity of 105.3 mAh g −1 at 2.0 A g −1 and good cycling lifespan. The present study offers a homologous design strategy based on PB and its derivatives for constructing outstanding sodium-ion full cells.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2019 · IF 7.467

Morphology regulation of Li2O2 by flower-like ZnCo2S4 enabling high performance Li-O2 battery

Zhiqian Hou,Shan Feng,Peng Hei,Tingshuai Yang,Zhiqun Ran,Ruixin Zheng,Xin Liao,Chaozhu Shu,Jianping Long

The development of high-efficiency oxygen electrode with well structural and chemical stability is critical to boost the rapid development of lithium-oxygen (Li-O 2 ) batteries. Which are reckoned as a potent contender for next-generation energy storage devices due to their ultra-high theoretical energy density . Here, a flower-like three-dimensional self-standing ZnCo 2 S 4 -based electrode without an addition of binders are fabricated and employing as positive electrode for Li-O 2 batteries. The bifunctional catalytic activity of flower-like ZnCo 2 S 4 is conducive to improving the hysteresis kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Representative ultrathin petal edge exposes adequate active sites and provides a sufficient contact interface between Li 2 O 2 and positive electrode, which are essential for reducing the charge overpotential during OER. Compared with the control electrodes, the flower-like ZnCo 2 S 4 @Ni-based Li-O 2 battery shows decreased overpotential (0.78 V) and improved cycle stability (over 500 cycles).

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2019 · IF 5.383

Preparation of pyridine N-doped metal-free Li–O2 battery cathode by one-step

Hongyu Dong,Ke Li,Yiwen Wang,Yanhong Yin,Shuting Yang

Lithium-oxygen (Li–O 2 ) batteries are an ideal energy storage device, but the problems of the cathode still hinder their development. In this work, a metal-free, binder-free and in situ pyridine N-doped cathode of Li–O 2 batteries is synthesized in one step by electrospinning. Meanwhile, the effect of carbonization temperature on cathode is discussed in detail. The content of pyridine N in the cathode is the highest at the carbonization temperature of 700 °C, and it is also the most effective for the reversible formation and decomposition of Li 2 O 2 . In terms of Li–O 2 batteries performance, when the charge and discharge current density is 100 mA g −1 and the discharge voltage is greater than 2 V, the discharge specific capacity and discharge capacity can reach 27900 mAh g −1 and 27.9 mAh respectively. In addition, when the limited specific capacity is 1000 mAh g −1 , the batteries can work stably for 85 cycles under the same conditions. Therefore, the high-performance cathode which synthesized in one step by electrospinning is expected to promote the commercial application of Li–O 2 batteries.

研究领域: 材料科学 · 能源存储技术
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Molten Salt Thermal Treatment Synthesis of S-Doped V2CTx and Its Performance as a Cathode in Aqueous Zn-Ion Batteries

Weiyan Jiang,Huizhong Shi,Miao Shen,Rui Tang,Zhongfeng Tang,Jian-Qiang Wang

The lack of suitable cathode materials with a high capacity and good stability is a crucial problem affecting the development of aqueous Zn-ion batteries. Herein, a novel strategy for the modification of V2CTx through molten salt thermal treatment is proposed. In the novel route, S heteroatoms were introduced into V2CTx through a substitution reaction during the dissolution of Li2S in LiCl–KCl molten salts. Then, surface V2O5 was obtained through the in situ electrochemical charging/discharging of the S-doped V2CTx (MS-S-V2CTx) cathode. The assembled Zn/MS-S-V2CTx battery showed a high reversible discharge capacity of 411.3 mAh g–1 at a current density of 0.5 A g–1, an 80% capacitance retention after long cycle stability tests at 10 A g–1 for 3000 cycles, and a high energy density of 375.5 Wh kg–1 in 2M ZnSO4. Density functional theory calculations demonstrate that the improved electrochemical performance of the cathode can be attributed to the introduced S heteroatoms, which considerably reduced the ion diffusion energy barrier for Zn2+ ions and improved the stability of V2O5. This work provides a novel method to produce highly active and stable vanadium-based cathodes for aqueous Zn-ion batteries.

研究领域: 材料科学 · 电化学 · 储能技术
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Polymers · 2024 ·Vol. 16 ·期 23 ·3276 · IF 4.7

Polypyrrole-Derived Nitrogen-Doped Tubular Carbon Materials as a Promising Cathode for Aqueous Aluminum-Ion Batteries

Xiaoming Zhou,Xiaolei Li,Jiaming Duan,Lihao Zhang,Xinyu Mo,Qing Wu,Yang Liu,Guohui Yuan,Miaosen Yang

The advantages of aluminum-ion batteries in the area of power source systems are: inexpensive manufacture, high capacity, and absolute security. However, due to the limitations of cathode materials, the capacity and durability of aluminum-ion batteries ought to be further advanced. Herein, we synthesized a nitrogen-doped tubular carbon material as a potential cathode to achieve advanced aqueous aluminum-ion batteries. Nitrogen-doped tubular carbon materials own an abundant space (367.6 m2g−1) for electrochemical behavior, with an aperture primarily concentrated around 2.34 nm. They also exhibit a remarkable service lifespan, retaining a specific capacity of 78.4 mAh g−1at 50 mA g−1after 300 cycles. Additionally, from 2 to 300 cycles, the material achieves an appreciable reversibility (coulombic efficiency CE: 99.7%) demonstrating its excellent reversibility. The tubular structural material possesses a distinctive hollow architecture that mitigates volumetric expansion during charging and discharging, thereby preventing structural failure. This material offers several advantages, including a straightforward synthesis method, high yield, and ease of mass production, making it highly significant for the research and development of future aluminum-ion batteries.

CAS / MDL: 7446-70-0
研究领域: 材料科学 · 电化学 · 能源存储
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ENERGY & FUELS · 2024 · IF 5.2

Green and Sustainable Recovery of MnO2 from Alkaline Batteries for High-Performance Lithium Manganese Oxide Cathode

Yunkai Xu,Keyang Qian,Yongjin Deng,Zixuan Liu,Zhengfei Chen

Massive spent Zn-MnO2 primary batteries have become a mounting problem to the environment and consume huge resources to neutralize the waste. This work proposes an effective recycling route, which converts the spent MnO2 in Zn-MnO2 batteries to LiMn2O4 (LMO) without any environmentally detrimental byproducts or energy-consuming process. The recycled LMO shows a pure phase and high-crystallinity properties, and more importantly, when used as lithium-ion cathodes, the recycled LMO exhibits impressive reversible capacity of 111.9 mAh g–1 and excellent cycling stability with 88.3% capacity retention after 500 cycles. Such recycling strategy not only solves the massive spent battery problems with its sustainable process but also transforms the waste (spent MnO2) into valuable assets (LIB cathodes).

CAS / MDL: 7722-84-1
研究领域: 环境科学 · 材料科学 · 能源科学
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Sustainable Materials and Technologies · 2024 · IF 8.6

Innovative green intense tetra-eutectic solvent (ITES) for recovery via occlusion co-precipitation at room temperature

Md Mofasserul Alam,Haijian Huang,Zeheng Yang,Lei Zou,Ziwei Chi,Weixin Zhang

Lithium iron phosphate (LiFePO 4 ) is the widely used cathode material for safe and high-power lithium-ion batteries (LIBs) for electric vehicles (EVs). Therefore, numerous challenges to re-manufacturing, re-use, and recovery from spent LiFePO 4 /C are tolerated if evaluated early in the innovation process. Herein, innovative green intense tetra-eutectic solvent (ITES) has been used to recover a new Li-metal co-intercalation compound from spent LiFePO 4 /C cathode material, which is simple and cost-effective. The ITES leaching concerning organic solution with active hydrogen donor-acceptor salts creates a coordination environment through occlusion co-precipitate new co-intercalation compound at room temperature. Innovative green ITES-10 solution has successfully recovered a new Li-metal co-intercalation regarding the active hydrogen donor-acceptor bonding coordination environment of ITES adequate leaching solution and proposed recovery mechanism. The ICP-MS value of recovery metal ( 7 Li) efficiency (%) of ITES-10 leaching for spent LiFePO₄/C cathode materials reaches approximately 0.452% at room temperature for recovery of new co-intercalation compound, besides the fresh LiFePO₄/C cathode materials (as reference), approximately 0.805%, respectively. Therefore, innovative ITES is considered to recover spent Li-based cathode materials in our future works concerning high leaching recovery rates below 100 °C in experimental conditions.

研究领域: 材料科学 · 环境科学 · 化学工程
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ACS Applied Energy Materials · 2024 · IF 5.4

Waterborne Acrylonitrile Copolymer Binder for 4.5 V High-Voltage Lithium Cobalt Oxide of Lithium-Ion Batteries

Leshuai Qiao,Yang Chen,Xuanxuan Zhang,Xiangxin Cheng,Wanfu Liang,Yuyu Li,Jingchao Chai,Ming Xie,Dianbo Ruan,Zhihong Liu

Water-based binders in lithium-ion batteries have garnered increasing attention owing to their environmental benignity and cost effectiveness. In this research, a waterborne poly(lithium acrylate-co-acrylonitrile) copolymer, P(LiAA-AN), was prepared and utilized as a high-performance binder for 4.5 V LiCoO2 in a lithium-ion battery. This copolymer binder integrates characteristics of both polyacrylic lithium and polyacrylonitrile. It has the ability to compensate for additional Li ions and engage in the formation of a stable cathode solid electrolyte interface (CEI) on the surface of 4.5 V LiCoO2. Consequently, in comparison with poly(vinylidene fluoride) (PVDF) and LiPAA binders, the water-based P(LiAA-AN) binder leads the 4.5 V LCO/Li battery to superior rate performance and high cycle stability. When the cell was cycled under a current density of 0.5 C (1 C = 185 mAh g–1) and a cutoff voltage of 3.0–4.5 V (vs Li+/Li), a high capacity retention ratio of 91.5% was achieved after 200 cycles. In addition, the P(LiAA-AN) binder demonstrates an excellent electrolyte absorption and a reduced charge transfer impedance. These results substantiate the effectiveness of the P(LiAA-AN) water-based binder in enhancing the electrochemical performance of the high-voltage LiCoO2 cathode.

研究领域: 材料科学 · 电化学 · 能源存储
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Journal of Energy Storage · 2024 · IF 8.9

Ultrafast preparation of LiNi0.5Co0.2Mn0.3-xMgxO2 cathode materials by a facile microwave reaction

Yongshun Liang,Haiyang Liu,Ya Li,Lang Xu,Yiyao Li,Yingjiao Yang,Wei Bai,Junming Guo,Mingwu Xiang

LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM) layered oxide is recognized as a promising cathode material of lithium ions battery and generally synthesized using a co-precipitation reaction to firstly obtain hydroxide precursors following by high-temperature solid method. The co-precipitation has the relatively complex and time-consuming process, whilst showing the nonuniform lithium distribution when mixed with spherical hydroxide precursors. Herein, a facile one-step microwave method is proposed to fast synthesize various LiNi 0.5 Co 0.2 Mn 0.3-x Mg x O 2 (x ≤ 0.05) cathode materials at a microwave power of 720 W only for 5 min. And then traditional solid method is used to further enhance the crystallinity and reduce the Li + /Ni 2+ mixing of the LiNi 0.5 Co 0.2 Mn 0.3-x Mg x O 2 samples. The as-prepared LiNi 0.5 Co 0.2 Mn 0.3-x Mg x O 2 samples have analogous polyhedral morphology and uniform element distribution. Also, the substitution of appropriate Mg-doping for Mn element boosts the stable layered structure and facilitates the Li + ions diffusion. Owing to these merits, the optimized LiNi 0.5 Co 0.2 Mn 0.27 Mg 0.03 O 2 cathode material exhibits a higher capacity retention of 87.90 % than that of the pristine LiNi 0.5 Co 0.2 Mn 0.3 O 2 sample (78.12 %) after 100 cycles at 0.2C.

研究领域: 材料科学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2014 · IF 2.726

Facile synthesis of hollow carbonized polyaniline spheres to encapsulate selenium for advanced rechargeable lithium–selenium batteries

Jie Li,Xingxing Zhao,Zhian Zhang,Yanqing Lai

A hollow carbonized polyaniline spheres/selenium (HCPS/Se) composite was prepared by a simple combination method of a self-assembly method, pyrolysis and vapor phase infusion process as a cathode material for Li–Se rechargeable batteries. The composites were characterized and examined by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, the X-ray photoelectron spectroscopy and electrochemical methods, such as cyclic voltammetry, electrochemical impedance spectroscopy and galvanostatic charge/discharge tests. The HCPS/Se composite cathode can deliver relative high capacity, high Coulombic efficiency and good cycling performance. The electrochemical results show that the HCPS/Se composite cathode exhibits an initial discharge specific capacity of 571.5   mA   h   g −1 and retains 298.7   mA   h   g −1 with high Coulombic efficiency after 100 cycles at a high rate of 0.5   C (337.5   mA   h   g −1 ), which are higher than that of the pristine selenium cathode. The excellent electrochemical properties benefit from the high conductivity and the hollow structures of the carbonized polyaniline spheres.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 电池技术
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

Facile synthesis of crack-free single-crystalline Al-doped Co-free Ni-rich cathode material for lithium-ion batteries

Qi Liu,Zhenqian Wu,Jingying Sun,Ruimei Xu,Xianwei Li,Xiao Yu,Yong Liu

Co-free, Ni-rich cathode materials have aroused enormous attentions for the low cost, sustainable development of lithium-ion batteries. However, it is not easy to fabricate single-crystalline Ni-rich cathode materials from the hierarchical structured precursors via coprecipitation method. Furthermore, it is difficult to introduce Al dopant during the coprecipitation process to obtain high quality Ni-rich cathode material owing to the rapid sediment of Al 3+ . Herein, we developed a one-step stirring-assisted cation chelation and reassembly route for fabricating crack-free single-crystalline, Al-doped Co-free Ni-rich cathode material. The fabricated LiNi 0.8 Mn 0.16 Al 0.04 O 2 shows a high capacity of 204 mAh g −1 at 0.1C, excellent rate capability (143 mAh g −1 at 10C), and good cycling stability (an initial specific capacity of 178 mAh g −1 with capacity retention of 82.2% at 1C over 200 cycles). Furthermore, when tested at a raised temperature of 55 °C, it exhibited an initial capacity of 194.7 mAh g −1 with capacity retention of 82.1% at 1C over 100 cycles. The outstanding electrochemical performance can be ascribed to the synergistic effect of single crystalline structure and successful doping of Al element in the cathode, which enable fast ion and electron transport , suppress Li/Ni mixing and maintain the structural stability.

研究领域: 材料科学 · 电化学 · 能源存储技术
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