SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Bingheng Liang,Xiaoya Gao,Qingcun Gu,Xuhao Liu,Teng Guo,Jiatian Wang,Wenjie Zhu,Yongming Luo
Increasing number of spent lithium-ion batteries (LIBs) presents opportunities and challenges for the recycling of cathode LiCoO 2 (LCO). Here, simultaneously selective leaching Li and fabricating cobalt oxide catalyst was developed by autocatalytic Peroxymonosulfate (PMS) advanced oxidation method at ambient temperature without strong acids. Where, superoxide radical ( O 2 · - ) was generated to break Li-O leaching 96.6 % of Li, and induced part conversion of Co 3+ to Co 2+ forming oxygen vacancies (O V ) in the remaining Co-containing product (NLCO). Compared with LCO (without delithiation), NLCO promoted greater electron transfer to activate PMS producing radical ( SO 4 · - and •OH) and non-radical ( 1 O 2 and Co(Ⅳ)=O) in the degradation of emerging pollutants (carbamazepine, CBZ). Hence, the NLCO/PMS system was effective in removing CBZ with resistance to pH variation and water matrix interference ( SO 4 2- , NO 3 - , and HA). COHP calculation results revealed the strong and almost unbreakable Co-O in NLCO, with significantly low Co leaching ensuring the excellent stability (100 % degradation activity maintained after 7th cycling) for removing pollutants in the liquid-phase reaction. Degradation pathways and toxicity analysis elucidated that the NLCO/PMS was a green and toxicity reduction process for removing CBZ. This study showcased a novel method for recovering Li from spent LCO and subsequently producing an environmental catalyst form spent LIBs.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
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2023
·Vol. 11
·期 18
·9913-9921
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IF 11.9
Longhao Cao,Hui Wang,Ziyin Guo,Jing Zhang,Xiaosong Zhang,Cancan Peng,Jingxiong Yu,Ya-Jun Cheng,Yonggao Xia
LiCoO2 (LCO) has attracted wide attention due to its high energy density, whose synthesis relies on the cobalt oxide precursor. The conventional synthetic method features a low yield. What is even worse, order–disorder phase transition of LCO occurs above 4.2 V, leading to structural instability and rapid capacity decay. To tackle these problems, a new synthetic method is proposed in this work, where LiCoO2 is in situ formed using cobalt metal as the precursor. M-LCO-850 °C (cobalt metal used as the precursor) exhibits a better cycle performance and faster Li+ diffusion rate than C-LCO (commercial synthesis method). The stable cycling performance is associated with the suppression of the order–disorder phase transition, which is attributed to the Co2+ “pillar” effect. Co2+ occupies the Li layer in the charge and discharge process, which acts as a “pillar” to support the CoO2 layer to inhibit order–disorder phase transition during the cycle, reducing the polarization and promoting the insertion/de-insertion reaction of Li+. Meanwhile, the synthesis yield and compacted density of M-LCO-850 °C are improved by 18.8% and 11.89%, respectively, compared to C-LCO. This method provides a new strategy for the in situ synthesis of cathode materials for lithium-ion batteries.
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Hao Guo,Zijun Min,Ying Hao,Xu Wang,Jinchen Fan,Penghui Shi,Yulin Min,Qunjie Xu
Increasing demand and waste of lithium-ion batteries (LIBs) has adversely affected resources and the environment. Multistage utilization of spent LIBs is essential to their sustainable development. Here, we propose a simple recycling method of LiCoO 2 cathode scrap, based on the first use of the cathode scrap as a catalyst to degrade organic pollutants via peroxymonosulfate activation , and subsequent recovery of valuable metals from the used catalyst. Compared with pristine LiCoO 2 , the LiCoO 2 cathode scrap exhibits excellent catalytic performance due to the active sites generated, such as the vacancy generation and electronic structure modulation by the degradation of LiCoO 2 during the continuous lithiation and delithiation processes. The removal efficiency of cathode scrap to the o -phenylphenol exceeds 98% within 60 min, and the degradation efficiency is still above 95% after the 10th use because its unique sandwich and porous structure ensure the stability and recyclability . After multiple catalytic reactions, due to the generation of crack, the separation of the sandwich structure, and further degradation of active materials, the leaching efficiency of transition metals from the cathode scrap in deep eutectic solvent is promoted. 86% of lithium and 95% of cobalt are leached from the used catalyst respectively. This study provides a promising strategy for the sustainable development of LIBs and promotes the utilization of spent LIBs in multiaspect.
研究领域:
环境科学
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材料科学
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可持续发展
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Zhen Sun,Yanqing Lai,Na lv,Yaqi Hu,Bingqin Li,Liangxing Jiang,Jiong Wang,Shuo Yin,Kui Li,Fangyang Liu
Argyrodite sulfide solid electrolytes, such as Li6PS5Cl (LPSC), have received much attention due to their high ionic conductivity (>1 mS cm–1) and success in all-solid-state batteries (long cycle performance, high energy density, etc.). Numerous efforts are spent on modifying the properties of the electrolyte itself. Here, we combine first-principles calculations with experiments to investigate O-doped argyrodite sulfide solid electrolytes (Li6PS5–xClOx,x = 0–1). It is found that Li6PS4.75ClO0.25 (LPSCO0.25) with x = 0.25 and cubic phase (F4̅3 m) shows the highest ion conductivity of 4.7 mS cm–1 (cold-pressed), higher than that of undoped Li6PS5Cl (4.2 mS cm–1). The bare LiCoO2/LPSCO0.25/Li–In all-solid-state battery exhibits an initial capacity of 131 mA h g–1 at 0.1 C and satisfactory cycling stability with 86% capacity retention after 250 cycles to the 4th cycle at 0.3 C under 25 °C. In addition, the NCM811/LPSCO0.25/Li–In cell is assembled using bare LiNi0.83Co0.06Mn0.11O2 cathode and shows an initial discharge capacity of 181 mA h g–1 at 0.1 C and 160 mA h g–1 at 0.3 C. The doping of oxygen-forming Li6PS5–xClOx also improves the stability to Li metal, proven by cyclic voltammetry and powder X-ray diffraction tests. The calculation results for the band structure reveals that LPSC has the lowest unoccupied molecular orbital than LPSCO0.25, further confirming the above conclusion.
研究领域:
材料科学
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电化学
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能量存储
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DOI
高影响因子
Small
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2024
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IF 13
Qian He,Xiongxiong Liu,Guang Xiao,Xuhua He,Wenbin Gong,Lingfei Tang,Qi Chen,Qichong Zhang,Yagang Yao
All-solid-state lithium metal batteries (ASSLMBs) have emerged as the most promising next-generation energy storage devices. However, the unsatisfactory ionic conductivity of solid electrolytes at room temperature has impeded the advancement of solid-state batteries. In this work, a multifunctional composite solid electrolyte (CSE) is developed by incorporating boron nitride nanotubes (BNNTs) into polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP). BNNTs, with a high aspect ratio, trigger the dissociation of Li salts, thus generating a greater population of mobile Li + , and establishing long-distance Li + transport pathways. PVDF-HFP/BNNT exhibits a high ionic conductivity of 8.0 × 10 −4 S cm −1 at room temperature and a Li + transference number of 0.60. Moreover, a Li//Li symmetric cell based on PVDF-HFP/BNNT demonstrates robust cyclic performance for 3400 h at a current density of 0.2 mA cm −2 . The ASSLMB formed from the assembly of PVDF-HFP/BNNT with LiFePO 4 and Li exhibits a capacity retention of 93.2% after 850 cycles at 0.5C and 25 °C. The high-voltage all-solid-state LiCoO 2 /Li cell based on PVDF-HFP/BNNT also exhibits excellent cyclic performance, maintaining a capacity retention of 96.4% after 400 cycles at 1C and 25 °C. Furthermore, the introduction of BNNTs is shown to enhance the thermal conductivity and flame retardancy of the CSE.
研究领域:
材料科学
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电化学
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能源存储
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纳米技术
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Yi-Feng Liu,Hong-Rui Wang,Jiang-Yu Li,Meng-Jie Chen,Hui Chen,Bing-Yi Lu,Qiang Ma,Xiong-Wei Wu,Xian-Xiang Zeng
The lithium (Li) metal battery reveals appealing merits in energy density but suffers from problems of dendrite growth and low coulombic efficiency before its applications. The ether electrolytes entitle Li metal batteries with more smooth Li stripping/deposition but narrow electrochemical stability in contrast to carbonate electrolyte. circumventing this contradictory, a lithium fluoride-nitride mixed ionic conducting interphase was embedded on lithium surface via formulated fluorine-rich carbonate and cyclophosphonitrile, which renders a dendrite-free plating/stripping over 2200 h and extend the electrochuemcial window of ether electrolyte to 4.5 V with the assistance of experiments and calculating simulations, ensuring LiCoO 2 to operate efficiently over 200 cycles with nearly no capacity decay.
研究领域:
材料科学
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电化学
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电池技术
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Honghu Li,Nuoya Chen,Weifeng Liu,Huazhang Feng,Jingyun Su,Dongju Fu,Xuguang Liu,Mingxia Qiu,Luyang Wang
The prosperity of the lithium-ion battery industry has raised deep concerns about spent batteries. Recently, much attention has been focused on the development and advancement of lithium battery recycling. Deep eutectic solvents are efficient, environmentally friendly, and economical leaching solvents with great potential for the recovery of cathode materials from spent lithium-ion batteries. However, to date, deep eutectic solvents have been considered a disposable agent for lithium-ion battery recycling, resulting in organic waste after a single recycling. Here, we demonstrate a reusable deep eutectic solvent based on maleic acid (MA) and ethylene glycol (EG), designed to recycle LiCoO 2 cathode materials from spent lithium-ion batteries. With a high loading capacity (59 g/L), the leaching efficiencies of Co and Li by MA:EG are 98.3 % and 98.4 % respectively. MA:EG can be refreshed by adding oxalic acid as a precipitant. Even after 4 cycles, the leaching efficiency of Co is still 90 % and the average recovery efficiency of Co products is over 96.5 %. Lithium is present in a high concentration and is also recovered in the form of oxalate. This work provides a novel and environmentally friendly recycling route that can economically and efficiently recover the valuable metals Li and Co from spent lithium-ion batteries.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
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IF 2.7
Yichuan Kong,Yongzhi Duan,Yuezhi Zhang,Yulin Min,Hongxiu Lu,Penghui Shi
The lithium-ion battery industry is experiencing explosive growth. Efficiently and greenly recycling Li, Co and other valuable metals is extremely important to alleviate the scarcity of resources and protect the environment. In this study, an improved recycling strategy is proposed to convert spent LiCoO2 batteries into water-soluble sulfate below 350 °C using the auxiliary effect of urea on sulfation roasting. This strategy not only allows for the direct synthesis of precursors for regeneration after selective recovery of lithium and cobalt but also further reduces the roasting temperature requirement compared to the conventional salt-thermal method. After roasting, Li and Co can be recovered from the solution by simple aqueous leaching. Under optimal conditions, the leaching rates of Li and Co were 94.94% and 95.47%, respectively. Subsequently, the Li and Co compounds that could be used as battery precursors were obtained by the addition of CO32−. Characterized by high efficiency, low energy consumption, absence of secondary pollution, and utilization of inexpensive and readily accessible raw materials, this approach offers a novel concept in the domain of lithium-ion battery recycling via salt-thermal methods.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Energy Storage Materials
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2024
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IF 18.9
Laibing Luo,Kean Chen,Ruoyu Cao,Hui Chen,Miaomiao Xia,Along Zhao,Xiaoyang Chen,Weihua Chen,Zhongxue Chen,Yongjin Fang,Yuliang Cao
Lithium-ion batteries (LIBs) operating at low temperature has always been a significant challenge. In this work, Ethyl fluoroacetate (EFA) was utilized as a single solvent to design a low-temperature electrolyte (LTE). The weak Li + -solvent interaction facilitates fast de-solvation process and improved low-temperature performance, while the high oxidation resistance and fluorine-rich electrolyte/electrolyte interface induced by the fluorinated groups enables wide operating voltage and stable cycling of the LIBs . The EFA-based electrolyte endows the high-voltage (4.45 V) Graphite//LiCoO 2 pouch cell with prominent low-temperature adaptability (89.7 % capacity retention retains at −40 °C, and capable of charging at −20 °C) and outstanding cycling performance (87.7 % capacity retention after 400 cycles). This work sheds light on the design of high-voltage and low-temperature electrolytes for lithium-ion batteries.
研究领域:
材料科学
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电化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2015
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IF 6.723
Yinan Zhao,Yujing Sha,Qian Lin,Yijun Zhong,Moses O Tade,Zongping Shao
Coarse-type LiCoO2 is the state-of-the-art cathode material in small-scale lithium-ion batteries (LIBs); however, poor rate performance and cycling stability limit its large-scale applications. Here we report the modification of coarse-type LiCoO2 (LCO) with nanosized lithium lanthanum titanate (Li3xLa2/3–xTiO3, LLTO) through a facile sol–gel process, the electrochemical performance of commercial LiCoO2 is improved effectively, in particular at high rates. The crystalline structure of pristine LiCoO2 is not affected by the introduction of the LLTO phase, while nanosized LLTO particles are likely incorporated into the space of the LiCoO2 layers to form a LCO-LLTO nanocomposite, which separate the LCO layers with the increase of layer spacing to ∼100 nm. The LLTO incorporation through the facile post-treatment effectively reduces the charge-transfer resistance and increases the electrode reactions; consequently, the LLTO-incorporated LCO electrode shows higher capacity than LiCoO2 at a higher rate and prolonging cycling stability in both potential ranges of 2.7–4.2 V and 2.7–4.5 V, making it also suitable for high-rate operation. This novel concept is general, which may also be applicable to other electrode materials. It thus introduces a new way for the development of high rate-performance electrodes for LIBs for large scale applications such as electric vehicles and electrochemical energy storage for smart grids.
研究领域:
材料科学
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电化学
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储能
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纳米材料
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电池技术
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DOI
高影响因子
Materials Today Energy
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2022
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IF 9.257
Qipeng Zhang,Nana Zhang,Tianhao Yu,Juyan Zhang,Bohua Wen,Lan Zhang
Solid-state lithium metal batteries (SSBs) have attracted ever-increasing attention because of the enhanced energy density and safety. However, the solid-solid contact resistance and interfacial stability pose a huge challenge in the practical application of SSBs. In this work, poly(acrylic acid) (PAA) is coated onto the LiCoO 2 (LCO) cathode surface via a simple drop-casting method in SSB employing poly(ethylene oxide) (PEO)-based electrolyte to construct an artificial cathode electrolyte interface (ACEI). It proves that the ACEI can not only form percolating Li + pathways across the electrode, but also protect the PEO electrolyte from being oxidized. Besides, Li + /H + exchange reaction is found between LCO and PAA during the initial cycles, which further promote the interfacial ion transport and lead to enhanced battery kinetics. Galvanostatic charge/discharge and electrochemical impedance spectroscopy test indicate that the 0.5% PAA-treated LCO presents superior capacity retention of 93.3% after 120 cycles at 0.4 C when it works at 60 °C. PAA-LCO|PEO|Li pouch cells are also prepared and a reversible capacity of 145 mAh/g after 50 cycles at 0.1 C is achieved, which further demonstrates the feasibility of this strategy.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
WASTE MANAGEMENT
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2026
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IF 7.3
Jiayi Wang,Shuqi Ren,Ruili Liang,Weijian Sun,Jianwen Xu,Yachao Jin,Mingdao Zhang,Li Song
An innovative suspension electrolysis method is proposed for LiCoO 2 recycling. • The electrolysis process can leach aqueous Li ions while generate solid Co oxide. • Direct regeneration of LCO is achieved via a closed-loop solid-state sintering. • Regenerated LCO restored comparable electrochemical properties to commercial LCO. • This strategy is scalable for mass production of industrial LiCoO 2 black mass. An innovative and green anodic “suspension electrolysis” strategy is designed for lithium extraction from industrial spent LiCoO 2 “black powders”, without additional acid, base or oxidizing/reducing agents required. As thoroughly illustrated by the electrolytic mechanism, Li ions driven by the electric energy are leached into the electrolyte while lithium-deficient Li x CoO 2 can be acquired as the anodic residual powders. The electrolysis process achieves an outstanding Li leaching efficiency of 92.1% and the Li ions can be recycled in the form of Li 2 CO 3 through a precipitate reaction by Na 2 CO 3 . The post-produced cobalt oxide and Li 2 CO 3 can be subjected to a solid-phase heat treatment for the regeneration of layered LCO. The regenerated LCO exhibits a discharge specific capacity of 149 mAh/g at 0.5 C, covering around 98.4% of the commercial LCO, and the capacity retention rate reaches up to 91.6% after 200 cycles at 0.5 C. This work provides an eco-friendly and scalable solution for recycling and regenerating spent LCO cathode materials. Download: Download high-res image (151KB) Download: Download full-size image
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DOI
PubMed
高影响因子
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