AICHE JOURNAL
·
2026
·
IF 4.4
Qian Liu,Xinze Yang,Yuxin Qiu,Xiangyi Kong,Hongye Cheng,Zhen Song,Zhiwen Qi
The recovery of cathode materials from spent lithium-ion batteries (LIBs) is highly beneficial for environmental protection and resource circularity. Here, an efficient closed-loop process is proposed for recycling spent LiCoO 2 . A novel deep eutectic solvent (DES) composed of betaine hydrochloride and pyruvic acid is proposed to achieve rapid and efficient leaching of Li and Co under mild conditions. Leaching kinetics of the DES is analyzed using the shrinking core model, while the leaching mechanism is systematically investigated by integrating experimental and theoretical approaches. Co and Li are recovered from the leachate through precipitation, and the leaching performance of the regenerated DES is also examined. The electrochemical performance of the regenerated LiCoO 2 is tested and compared with commercial LiCoO 2 . Finally, the economic and environmental analysis of the closed-loop recovery process is studied to evaluate its application prospects. This work provides valuable guidance for the comprehensive recycling and utilization of spent LIBs.
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高影响因子
ChemSusChem
·
2025
·Vol. 18
·期 15
·e202500148
·
IF 6.6
Chong Ni,Xuyong Feng,Yuanyun Dou,Wentao Wu,Hongfa Xiang
Surface coating is an efficient way to reduce side reactions between cathode materials and electrolytes, thus enhancing the cycle stability of cathode materials. In this study, a novel surface-coating strategy based on the melt curing process is introduced, which forms an ionic conductive LiAlO 2 layer on the surface of LiCoO 2 /LiNi 0.5 Mn 1.5 O 4 cathode materials and enhances the cycle stability of these cathode materials. Comprehensive characterizations, including scanning electron microscopy, energy dispersive spectrometer, and transmission electron microscopy (TEM) confirm the uniformity and thin LiAlO 2 coating. Electrochemical performance tests show better cycle performance of LiCoO 2 with 1% LiAlO 2 coating. An 85% capacity can be retained over 200 cycles at 1C and 4.5 V cutoff, compared to 61% for uncoated LiCoO 2 . For LiNi 0.5 Mn 1.5 O 4 , the coated sample shows 94.5% capacity retention after 300 cycles at 1C, while the capacity of the uncoated sample decays to 64.6% under the same condition. These findings underscore the effectiveness and universality of this surface-coating strategy. Graphical In this study, a novel surface-coating strategy based on a melt curing process is proposed, which forms an ion-conductive LiAlO 2 coating layer on the surface of LiCoO 2 cathode materials. TEM combined with EDS, XPS, etc. confirms the uniform thin layer LiAlO 2 coating, while the electrochemistry measurements prove the high stability of LiCoO 2 with LiAlO 2 coating.
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高影响因子
Energy Storage Materials
·
2021
·
IF 17.789
Xiao Wang,Qian Wu,Siyuan Li,Zheming Tong,Duo Wang,Houlong L. Zhuang,Xinyang Wang,Yingying Lu
Lithium cobalt oxide (LCO), a promising cathode with high compact density around 4.2 g cm −3 , delivers only half of its theoretical capacity (137 mAh g −1 ) due to its low operation voltage at 4.2 V (vs. Li/Li + ) under commercial conditions. To improve its practical capacity, higher cut-off voltages are often adopted, which result in severe structure destruction and cause side reactions with electrolyte. The safety concerns of oxygen release further restrict the application of LCO. Here, we achieve stable cycling of LCO at 4.6 V (vs. Li/Li + ) through a surface engineering strategy by using lithium-aluminum-phosphate composite coating materials . This strategy prevents direct contact between cathode and electrolyte, reducing the loss of active materials without hindering the lithium ion migration. After calcination , a doping layer (or solid solution) includes phosphorus and aluminum is formed, which helps maintain the surface structure and stabilize the oxygen atoms around particle surface and shows high ion mobility when operated at 4.6 V (vs. Li/Li + ). All these benefits synergistically contribute to the stable cycling of LCO at 4.6 V (vs. Li/Li + ) with high capacity retentions of 88.6% (30°C) and 78.6% (45°C), respectively, after 200 cycles.
研究领域:
材料科学
·
能源存储与转换
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Yonghao Huang,Zhangyating Xie,Weiya Zhu,Changyong Mo,Weishan Li,Youhao Liao
To solve the problems of narrow oxidation decomposition potential and low room temperature ionic conductivity of the traditional poly(ethylene oxide) (PEO)-based solid polymer electrolyte (SPE), a polycarbonate-based SPE is developed by facile in situ ultraviolet-irradiated polymerization for high-energy-density lithium metal batteries (LMBs). Since the weak complexation between carbonate groups and Li+-ions in the vinyl ethylene carbonate (VEC) section provides the ionic transport capability, while the rigid hydroxyethyl methacrylate (HEMA) segment facilitates the mechanical strengths, the prepared P(VEC-HEMA) copolymer-based SPE exhibits a high ionic conductivity of 0.8 × 10–3 S cm–1 at room temperature, an antioxidation potential exceeding 5.0 V, and a high Young’s modulus value of 2.3 GPa that can effectively prevent the puncture of lithium dendrites. Notably, the P(VEC-HEMA) copolymer presents a stronger binding energy with TFSI– than that of the PVEC oligomer, ascribed to the hydroxyl group in HEMA section that also gives a fast transport pathway for Li+-ions through hydrogen bonds. Contributed by the advanced functional groups inhered from distinct monomers, the assembled Li∥SPE∥LiCoO2 full cell using P(VEC-HEMA) electrolyte exhibits excellent rate capacity and long cyclic stability, which shows the specific discharge capacity of 138.1 mA h g–1 at 0.1 C rate in the voltage range of 3.0–4.2 V, maintaining 93.5% of initial capacity after 100 cycles. For comparison, the full cell using PVEC electrolyte has a short circuit after 13 cycles. Therefore, the proposed polycarbonate solid electrolyte gives a bright future to revitalize the development of high-energy-density LMBs.
研究领域:
材料科学
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电化学
·
电池技术
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Jie Wang,Yue Wang,Tong Tian,Xiaolin Song,Daochuan Jiang,Yupeng Yuan
Achieving high crystallinity in polymeric semiconductors is crucial for enhancing charge transport and optoelectronic performance. However, this remains a challenge due to the inefficiency of energy coupling during polymerization. Here, we introduce a precursor-polarization approach to improve the crystallinity of polymeric carbon nitride. By protonating the melem precursor, we generate highly polar -NH 3 ⁺ edge groups that significantly increase the microwave response and facilitate directional thermal activation during polycondensation. This polarization-mediated energy coupling accelerates the condensation process, yielding carbon nitride with improved crystallinity and charge transport properties. As a result, the material exhibits a tenfold increase in photocatalytic H 2 O 2 production compared with conventional microwave-generated carbon nitride, with an apparent quantum efficiency of 5.63% at 420 nm. Importantly, the photogenerated H 2 O 2 is directly applied to dissolve spent LiCoO 2 cathodes, demonstrating a solar-driven, environmentally benign strategy for lithium-ion battery recycling. This study establishes precursor polarization as a general design principle for controlling the crystallization of polymeric semiconductors and translating their optoelectronic advantages into sustainable chemical process.
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RSC Advances
·
2013
·Vol. 4
·期 20
·10196-10203
·
IF 2.562
Borong Wu,Yonghuan Ren,Daobin Mu,Xiaojiang Liu,Guchang Yang,Feng Wu
An electrolyte (LiPF6–EC/PC/DEC) containing a lithium carbonate (Li2CO3) additive is used to enable the high cycling stability of a lithium cobalt oxide (LiCoO2) cathode which is charged to 4.5 V for a higher capacity. A capacity as high as 162.8 mA h g−1 (1 C) is maintained after 116 cycles, which is twice as high as the capacity of 88.5 mA h g−1 which was achieved in the Li2CO3 free instance. The interface properties of the electrode are investigated by cyclic voltammetry, electrochemical impedance spectroscopy and X-ray photoelectron spectroscopy. It is found that the solid electrolyte interphase (SEI) film tends to be thin and steady, and that the electrolyte decomposition is suppressed with the addition of Li2CO3. A possible mechanism is proposed according to the DFT calculation. The results indicate that the Co4+…CO32− coordination may decrease the oxidizability of Co4+ on the electrode surface so that the electrolyte decomposition could be suppressed.
研究领域:
材料科学
·
电化学
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ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 22
·1909392
·
IF 16.836
Jiliang Qiu,Xinyu Liu,Rusong Chen,Qinghao Li,Yi Wang,Penghao Chen,Luyu Gan,Sang-Jun Lee,Dennis Nordlund,Yijin Liu,Xiqian Yu,Xuedong Bai,Hong Li,Liquan Chen
Poly(ethylene oxide) (PEO)-based solid electrolytes are expected to be exploited in solid-state batteries with high safety. Its narrow electrochemical window, however, limits the potential for high voltage and high energy density applications. Herein the electrochemical oxidation behavior of PEO and the failure mechanisms of LiCoO 2 -PEO solid-state batteries are studied. It is found that although for pure PEO it starts to oxidize at a voltage of above 3.9 V versus Li/Li + , the decomposition products have appropriate Li + conductivity that unexpectedly form a relatively stable cathode electrolyte interphase (CEI) layer at the PEO and electrode interface. The performance degradation of the LiCoO 2 -PEO battery originates from the strong oxidizing ability of LiCoO 2 after delithiation at high voltages, which accelerates the decomposition of PEO and drives the self-oxygen-release of LiCoO 2 , leading to the unceasing growth of CEI and the destruction of the LiCoO 2 surface. When LiCoO 2 is well coated or a stable cathode LiMn 0.7 Fe 0.3 PO 4 is used, a substantially improved electrochemical performance can be achieved, with 88.6% capacity retention after 50 cycles for Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 coated LiCoO 2 and 90.3% capacity retention after 100 cycles for LiMn 0.7 Fe 0.3 PO 4 . The results suggest that, when paired with stable cathodes, the PEO-based solid polymer electrolytes could be compatible with high voltage operation.
研究领域:
材料科学
·
电化学
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 18
·9913-9921
·
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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WASTE MANAGEMENT
·
2026
·
IF 7.3
Ruichao Zhu,Lin Chen,Jin Wu,Yixuan Zhou,Chuqing Cao,Liang Zhu,Longjie Jiang
Leaching of LCO using ferrous glycinate under ammonia leaching. • Achieved a high leaching efficiency for LCO. • Guaranteed the absence of non-target impurities in the final product. Efficient and environmentally sustainable recovery of valuable metals from spent lithium cobalt oxide (LiCoO 2 , LCO) cathodes is crucial for the lithium-ion batteries recycling. While ammonia leaching offers a promising pathway for green closed-loop recycling, its conventional application suffers from slow kinetics. To address this limitation, this study introduced ferrous glycinate (Gly-Fe) as a novel reductant, alongside FeCl 2 for comparison, into an NH 3 -based system, which enabled ultra-rapid reductive dissolution of LCO. A systematic investigation of key parameters, including temperature, ammonia concentration, and Fe/Co molar ratio, revealed Gly-Fe’s superior performance. It was found that nearly complete leaching efficiencies of Li + (∼100.0%) and Co 2+ (96.2% ± 2.1%) was achieved within just 60 min using Gly-Fe. In contrast, FeCl 2 attained Li + leaching of ∼ 100.0% but only 83.5% ± 2.6% for Co 2+ within 30 mins under comparable conditions, highlighting the kinetic advantage and effectiveness of the glycine-based complex. Noticeably, Fe 2+ from both reagents precipitated spontaneously in the alkaline ammonia medium without additional additives, facilitating the direct recovery of high-purity leach products. This approach preserved the intrinsic purity advantages of ammonia leaching while accelerating metal extraction rates and significantly enhancing metal recovery rates, thereby establishing a solid foundation for the development of efficient closed-loop recycling for spent lithium-ion batteries. Download: Download high-res image (107KB) Download: Download full-size image
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
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
·
材料科学
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高影响因子
Inorganic Chemistry Frontiers
·
2024
·
IF 6.1
Mengxiang Ye,Huaimeng Li,Xi Wu,Guofeng Zhang,Yunxia Zhang
Rapid rejuvenation and extensive utilization of mobile electronic devices lead to the excessive accumulation of waste lithium-ion batteries (LIBs), especially represented by spent LiCoO2 cathode materials. Considering the shortage of metals resources and the surging price of raw materials in the battery industry, it is in urgent demand to exploit an efficient strategy for selectively extract valuable metals from spent LiCoO2. Herein, the nanocube-like potassium zinc hexacyanoferrate (denoted as KZHCF) has been successfully fabricated on carbon cloth (CC) substrate for selective Co2+ adsorption from spent LiCoO2 cathode via the combination of simple electrodeposition and hydrothermal treatment. Under the optimal operational conditions, 98.6% of Co2+ is effectively extracted within 120 min at a constant potential of −0.4 V (vs. Ag/AgCl) with CC/KZHCF composite as working electrode, accompanied by a Co2+ electrosorption capacity of 130.9 mg∙g−1. Further, lithium ions in the electrolyte are separated and recovered in the form of Li2CO3 via simple chemical precipitation, highlighting the feasibility of the developed electrochemical system toward cobalt and lithium recovery. Significantly, the CC/KZHCF electrode materials can be regenerated through simple potential inversion; while the adsorbed Co2+ ions are facilely desorbed from the electrode surface and recovered as Co(OH)2. This work will provide a meaningful guidance for the separation and recovery of various metals from waste LIBs.
研究领域:
材料科学
·
环境科学
·
电化学工程
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高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Fengyin Zhou,Hongya Wang,Shiyu Wang,Jingjing Zhao,Xin Qu,Danfeng Wang,Yuqi Cai,Zhiyu Zheng,Dihua Wang,Huayi Yin
Waste biomass is one of the promising feedstocks to supply syngas that can be used as fuels, chemicals, reductants, etc. However, the relationship between the component of biomass and the constituent of pyrolysis gas remains unclear. Here, we study the pyrolysis behaviors of various biomasses and reveal the relationship between the biomass components and gas compositions. Further, different pyrolysis gases are applied for the reduction of spent lithium cobalt oxide (LiCoO2) below 500 °C. The pyrolysis gas with a higher concentration of CO has a higher reductivity to convert LiCoO2 to CoO and Li2CO3 with a conversion rate close to 100% in 1 h at 500 °C. The biomass rich in cellulose and with a lower content of lignin tends to produce pyrolysis gas with a high concentration of CO, which comes from the deliberate breakdown of carboxyl, carbonyl, ether, and ester linkages. Moreover, LiCoO2 exerts catalytic functions over the deoxygenation and enhancement of oxygenates and single-ring aromatics. Overall, this paper offers a tailored approach to regulating biomass pyrolysis gases, enabling highly efficient battery recycling and syngas production.
研究领域:
能源科学
·
环境科学
·
材料科学
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高影响因子
危险品化学品经营许可证（带存储）