JOM
·
2023
·Vol. 75
·期 9
·3632-3642
·
IF 2.6
Fei Zitong,Xing Yusen,Dong Peng,Meng Qi,Zhang Yingjie
The traditional direct regeneration of cathode material of spent lithium-ion batteries is encountering the challenge of high energy consumption. Here, an oxidative hydrothermal solution has been developed for direct regeneration of spent LiCoO 2 materials in low-temperature operation. The regenerated cathode material displays a better structural transformation with single-crystal particle morphology. More Co 2+ in spent LiCoO 2 materials are successfully transformed to Co 3+ in regenerated cathode materials. The initial discharge capacity of regenerated cathode materials reaches 153.46 mAh/g with a capacity retention rate of 95.02% after 200 cycles, which are both significantly higher than that of 39.83% in regenerated materials obtained by the traditional hydrothermal regeneration process. This oxidative hydrothermal solution can provide the electrochemical driving force to accelerate the repair of defects of spent cathode materials and break the limit of kinetics under low-temperature conditions. The low-temperature hydrothermal regeneration process is available to guide efficient and economically reasonable recycling of spent cathode materials.
研究领域:
材料科学
·
能源工程
·
环境科学
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DOI
高影响因子
Advanced Energy Materials
·
2022
·Vol. 13
·期 3
·2203703
·
IF 29.698
Wei He,Niaz Ahmad,Shaorui Sun,Xiao Zhang,Leguan Ran,Ruiwen Shao,Xuefeng Wang,Wen Yang
To implement the growing requirement for higher energy density all-solid-state lithium batteries (ASSLBs), further increasing the working voltage of LiCoO 2 (LCO) is a key to breaking through the bottleneck. However, LiCoO 2 severe structural degradation and side reactions at the cathode interface obstruct the development of high-voltage sulfide-based ASSLBs (≥4.5 V). Herein, a nano-metric Li 1.175 Nb 0.645 Ti 0.4 O 3 (LNTO) coated LCO cathode where microscopic Ti and Nb segregation at the interface during cycling potentially stabilizes the cathode lattice, and minimizes side reactions, simultaneously, is designed. Advanced transmission electron microscopy reveals that the stable spinel phase minimizes the micro stress at the cathode interface, avoids structure fragmentation, and hence significantly enhances the long-term cyclic stability of LNTO@LCO @ 4.5 V. Moreover, the differential phase contrast scanning transmission electron microscopy (DPC-STEM) visualizes the nano-interlayer LNTO to boost Li + migration at the cathode interface. Electrochemical impedance spectroscopy (EIS) reveals that sulfide-based cells with the LNTO nano-layer effectively reduce the interfacial resistance to 140 Ω compared to LiNbO 3 (235 Ω) over 100 cycles. Therefore, 4.5 V sulfide-based ASSLBs offer gratifying long-cycle stability (0.5 C for 1000 cycles, 88.6%), better specific capacity, and rate performance (179.8 mAh g –1 at 0.1 C, 97 mAh g –1 at 2 C).
研究领域:
材料科学
·
电化学
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DOI
高影响因子
CARBOHYDRATE POLYMERS
·
2026
·
IF 13.2
Yunyu Tong,Xinyue Zheng,En Chen,Zihan Guo,Rongfu Xu,Lulu Zhang,Zhaohui Wang
Raising the charging cutoff voltage of LiCoO 2 cathode is an effective route to boost the energy density of lithium-ion batteries. However, when operated above 4.5 V, LiCoO 2 electrode suffers from accelerated structural degradation and severe interfacial side reactions, leading to rapid capacity fading. Conventional PVDF binders offer limited protection under such high-voltage conditions due to their weak interfacial adhesion and chemical inertness, underscoring the need for more robust alternatives. Here, wood cellulose nanofibers are introduced as a multifunctional binder for high-voltage LiCoO 2 cathodes. Benefiting from its fibrous network and abundant functional groups, the cellulose binder forms a uniform, conductive coating that enhances Li + transport and suppresses electrolyte-induced degradation. As a result, the cellulose-based LiCoO 2 electrode delivers 91.1% capacity retention after 100 cycles at 4.6 V, significantly outperforming the PVDF counterpart. Moreover, material characterization confirms partial electro-degradation of the cycled cellulose binder, primarily through scission of glycosidic and carboxyl bonds. This work demonstrates the feasibility of employing aqueous nanocellulose binders for high-voltage cathodes and provides mechanistic insights to guide the molecular design of chemically stabilized cellulose materials for next-generation high-energy lithium-ion batteries.
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PubMed
高影响因子
Energy Storage Materials
·
2025
·
IF 20.2
Kai Zhang,Zeyu Wang,Zhenming Xu,Xing Zhou,Guodong Li,Zhe Mei,Yi Yu,Yonggang Wang,Congxiao Wang,Guannan Zhu,Yong-Ning Zhou,Yongyao Xia
Lithium cobalt oxide (LCO) has received considerable attention due to its high volumetric energy density, particularly at elevated cut-off voltages up to 4.7 V. However, the poor cyclic stability of high-voltage LCO limits its practical application, primarily due to detrimental phase transitions above 4.55 V, oxygen loss upon deep delithiation, and the interfacial side reactions. In this study, we introduce an in-situ formed strain buffer layer on LCO particles by CePO 4 coating to improve its high-voltage performance. The coated CePO 4 layer reacts with LCO particles spontaneously to generate a lattice-matched Li 8 CeO 6 phase, which can facilitate Li + transportation and relieve near-surface intrinsic stress. With less lattice strain, the undesirable phase transition and notorious surface degradation are suppressed significantly. Moreover, strong covalence of Ce 4f and O 2p bonds, and delocalized electrons in Ce-O 6 octahedral configuration help to suppress oxygen redox at 4.6 V. A high capacity retention of 93.3% after 300 cycles at 4.6 V and 88% after 100 cycles at 4.7 V is harvested. This strategy of constructing a strain buffer layer near the particle surface provides a novel insight for stabilizing the high-voltage LCO and paves the way for further modification of other cathode materials.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Advanced Science
·
2022
·Vol. 9
·期 11
·2104841
·
IF 17.521
Shulan Mao,Zeyu Shen,Weidong Zhang,Qian Wu,Zhuoya Wang,Yingying Lu
The energy density of batteries with lithium cobalt oxide (LCO) can be maximized by increasing the cut-off voltage to approach the theoretical capacity limit. However, it is not realized in the practical applications due to the restricted cycle life caused by vulnerable cathode surface in deep delithiation state, where severe side reactions, oxygen/cobalt loss and structure degradation often happen. Here, an outside-in oriented nanostructure on LiCoO 2 crystals is fabricated. The outer electrochemically stable LiF and Li 2 CoTi 3 O 8 particles perform as physical barrier to prevent damage of both cathodes and electrolytes, while the inner F doping promote Li ions diffusivity and stabilize the lattice oxygen. With the spinel-like transition layer between them, a solid and complete lithium-ion transport channel generation along the lithium concentration gradient. Under the protection from this structure, the LiCoO 2 withstand the high voltage of 4.6 V and the LCO/graphite pouch full cell with high loading density exhibits 81.52% energy density retention after 135 cycles at 4.5 V.
研究领域:
材料科学
·
储能
·
电化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Bin Ye,Mingzhi Cai,Miao Xie,Hang Dong,Wujie Dong,Fuqiang Huang
Improving the durability of cathode materials at low temperature is of great importance for the development nowadays of lithium ion batteries, since the practical capacity and cycling stability of the electrode are reduced significantly at low temperature. Herein, by amorphous Zr3(PO4)4 surface engineering, we realize a stable high-voltage LiCoO2 operation (4.6 V) at −25 °C. The highly amorphous surface layer can help to form a high-quality cathode-electrolyte interphase with strong stability and low interface resistance, especially at low temperature. Such a surface-engineered LiCoO2 shows a capacity of 179.2 mAh g–1 at 0.2C and an excellent cyclability with 91% capacity retention after 300 cycles (1C). As a comparison, bare LiCoO2 shows only 161.6 mAh g–1 and 1% capacity retention under the same circumstances. This work confirms that surface regulation and control engineering is an effective route to improve the high-voltage and low-temperature performance of LiCoO2.
研究领域:
材料科学
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电化学
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储能技术
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表面工程
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电池技术
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Bin Wang,Xin-Ye Lin,Yuanyuan Tang,Qiang Wang,Michael K.H. Leung,Xiao-Ying Lu
With the massive consumption of lithium-ion batteries in portable consumer electronics and electric vehicles, proper disposal of spent batteries is of paramount importance for sustainable development. In this study, biodegradable organic methanesulfonic acid (MSA) is investigated for the first time to leach valuable metals from waste LiCoO 2 powders for battery material regeneration. Under the optimal conditions, leaching efficiencies of lithium and cobalt are achieved at nearly ∼100% and ∼100%, respectively. Comparison experiment indicates that MSA can achieve better leaching performance than previously reported organic acids (e.g. citric acid , malonic acid , succinic acid , oxalic acid) under the same conditions. Besides, strong leaching capability of MSA at high solid-to-liquid ratios (e.g. 81.2 g L −1 and 163 g L −1 ) is confirmed with satisfactory leaching efficiencies (ca. 92.4%–100%). Feasibility test of MSA utilization for proper treatment of spent batteries is demonstrated at the optimized conditions. Importantly, regeneration study suggests that the as-obtained leachate can be employed to synthesize Co 3 O 4 anode and LiCoO 2 cathode materials with micro/nanostructures. Excellent cycling performance and rate capability of the regenerated electrode materials are demonstrated in the repeated charge-discharge cycles. Overall, the proposed recycling strategy is of great significance for rational resource utilization of spent lithium-ion batteries.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Suichang Ong,Huili Yang,Tu Lan,Kai Huang,Tianzheng Xie,Jinxia Zhou,Yuan Cheng,Hang Guo,Ying Zhang
Surface coating and element doping are the key strategies in LIBs development to achieve a high and stable battery performance. In this paper, ZrO 2 is directly sputtered on the Al-doped LiCoO 2 (Al-LCO) composite electrodes, enabling a controllable oxide coating on the surface of the electrode. With a sputtered coating layer of ∼6 nm, the discharging capacity of the Al doped LCO coated with ZrO 2 (Al-LCO-ZrO 2 ) is 141.04 mAh g −1 at the 100th cycle within 3.0–4.7 V at 1 C, while the Al-LCO (without coating layer) is 126.66 mAh g −1 . After 100 cycles of charging-discharging at high voltage region, the capacity retention of the Al-LCO-ZrO 2 -3 (90.7%) is also higher than the Al-LCO (75.57%). It is worth noting that, in this paper, due to the Al doping and the ZrO 2 coating, we increase the operation voltage up to 4.7 V, in which the batteries can obtain a higher energy density.
研究领域:
材料科学
·
能源技术
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2015
·Vol. 27
·期 44
·7150-7155
·
IF 17.493
Zhu Y,Zhou W,Chen Y,Yu J,Liu M,Shao Z.
Layered LiCo0.8 Fe0.2 O2 demonstrates dramatically enhanced oxygen evolution reaction (OER) activity and durability in an alkaline solution over LiCoO2 and other reported state-of-the-art catalysts, including benchmark IrO2 . This superior performance is attributed to Fe-doping-induced synergistic effects.
研究领域:
电化学
·
材料科学
·
催化
·
能源材料
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Zhanyi Jia,Peichen Yang,Yongqi Li,Denglei Gao,Jing Xia,Yijun Yang,Xi Wang,Yongan Yang
Elevating the charging cutoff voltage of lithium cobalt oxide (LiCoO2) batteries to 4.6 V (vs Li/Li+) enables the attainment of an impressive specific capacity; however, this advancement is hampered by severe structural degradation above 4.45 V attributed to unfavorable phase transitions and the occurrence of undesirable side reactions. Herein, we introduce high-valence Sb5+ into LiCoO2, suppressing the O3 to H1–3 phase transition and thereby enhancing the structural stability of LiCoO2. The stable structure not only enables the formation of a more stable cathode-electrolyte interphase film on the surface of LiCoO2 but also suppresses the dissolution of Co, reducing surface side reactions. As a result, Sb-doped LiCoO2, serving as a 4.6 V anode, exhibited a remarkable specific capacity of 169.2 mAh g–1 at a current density of 1C, with a durable capacity retention of 83.2% after 100 cycles. This study offers a structural modulation strategy for the further advancement of high-voltage LiCoO2 cathodes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Peng Wang,Zhuoli Yang,Chunxian Xing,Jiawei Huang,Guangren Wang,Yucheng Zhang,Da Guo,Mengdan Jiang,Lixi Zheng,Peng Yang,Tingfang Tian,Linfeng Fei
Abstract Current demands for recycling retired cathode materials and developing high-energy-density lithium-ion batteries inspire the possible conversion of end-of-life LiCoO2 (LCO) streams into next-generation high-voltage cathode materials. In this work, we demonstrate a one-step approach that upcycles degraded LCO materials by synergistically combining Mg/Al dual-doping with Li3PO4 surface engineering for stable high-voltage applications. The product demonstrates exceptional electrochemical performance up to 4.6 V, delivering 211.7 mAh g–1 at 0.1 C with outstanding cycling stability (98.56% and 80.21% capacity retention after 200 and 500 cycles at 1 C, respectively), far exceeding that of commercial LCO material (75.52% after 200 cycles); the superiority stems from the synergistic bulk-surface modification that simultaneously suppresses phase transitions and interfacial degradation during electrochemical operations. This work provides a transformative pathway for unlocking the high-voltage potential of LCO from degraded materials while demonstrating that rational material engineering well aligns environmental sustainability with enhanced electrochemical performance.
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DOI
高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Fengyin Zhou,Hongya Wang,Danfeng Wang,Shiyu Wang,Baolong Qiu,Xiang Chen,Dihua Wang,Lawrence Yoon Suk Lee,Huayi Yin
Spent LIB black mass is a highly heterogeneous mixture, and its compositional complexity remains a key barrier to efficient and sustainable circularity of energy materials. Here, we propose an enhanced gas-phase recovery route integrating pyrolysis-gas reduction with CO 2 -carbonated water leaching for LiCoO 2 black-mass recycling. Biomass-derived reducing gases, together with intrinsic graphite, cooperatively tune the reducing atmosphere, oxygen potential, and phase evolution, while graphite acts as an in situ carbon source to drive secondary gas equilibria and gas-solid reactions, reshaping the CO/CO 2 /H 2 /CH 4 composition and stabilizing Li as Li 2 CO 3 . Downstream, CO 2 -carbonated water enables selective Li dissolution via a reversible bicarbonate pathway, lowering water use and evaporation energy demand. An integrated electrochemical purification step rapidly removes trace dissolved Co from the carbonate leachate, supporting closed-loop operation and product purity. Validated using real smartphone black mass, the process delivers high recoveries (∼97%) of Li and Co as Li 2 CO 3 and Co 3 O 4 for LiCoO 2 batteries. This work offers energy-relevant insights for building low-energy, low-waste recycling pathways that improve material security and economic resilience. An integrated pyrolysis-gas reduction and CO 2 -carbonated water leaching strategy enables low-temperature, low-water recycling of spent LiCoO 2 black mass, achieving selective Li recovery and cleaner separation of Co-containing products. Download: Download high-res image (202KB) Download: Download full-size image
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高影响因子
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