JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Jingjing Zhao,Danfeng Wang,Fengyin Zhou,Hongya Wang,Xin Qu,Yuqi Cai,Zhiyu Zheng,Dihua Wang,Huayi Yin
The recycling of spent lithium-ion batteries (LIBs) is pivotal for advancing industrial resource sustainability and economic viability. However, conventional recovery processes face significant challenges, including excessive energy consumption, reagent overuse, and inefficiencies in material separation. Herein, a slurry electrochemical assisted method is proposed for co-recycling spent LiCoO 2 (LCO) and LiFePO 4 (LFP) enabled by their redox reactions. The redox reaction of LCO and LFP allows the leaching efficiency of Li to reach 99.4 % and Co to achieve 98.1 % at the conditions of 1 mol L −1 H 2 SO 4 and under a constant cell voltage of 3 V. Over the process, the dissolved Fe 2+ from LFP in the beginning plays a critical reduction role in destructing the stable structure of LCO. And the additional applied electricity reinforces the circulate of proton, thus enhancing the utilization rate of acid close to ∼99 %. More importantly, over 90 % of Fe 3+ is directly precipitated to FePO 4 ·2H 2 O without the precipitant additive. What's more, the relatively high solid-liquid ratio of 132.5 g L −1 simplifies the separation step and reduces process energy consumption. This study optimizes metal recovery efficiency through advanced electrochemical assisted co-leach and selective separation strategies, aiming to reconcile industrial scalability with circular economy goals.
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高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Min Li,Said Amzil,Cancan Peng,Xuan Ting Wu,Junwei Feng,Xingchen Liu,Jie Gao,Peter Müller-Buschbaum,Ya-Jun Cheng,Yonggao Xia
Lithium cobalt oxide (LCO) remains the predominant cathode for consumer electronics, owing to its superior volumetric energy density and theoretical capacity. However, extending its operating voltage beyond 4.5 V triggers aggressive electrolyte decomposition, leading to structural deterioration and rapid performance decay. To address this challenge, we propose a functionalized polyester-diacrylate-polydimethylsiloxane (PAPDMS) as a slurry additive, forming a protective layer. This layer plays a crucial role in improving electronic conductivity, enhancing mechanical flexibility, and facilitating electrolyte uptake of LCO. In particular, this protective layer not only modulates the solvation structure, thereby promoting the formation of an inorganic-rich CEI, but also effectively suppresses the dissolution of transition metals. The dual-effect synergy of the PAPDMS layer on both the electrode and electrolyte significantly enhances LCO stability at 4.5 V. Compared with the original LCO, the modified LCO shows an increase in capacity retention rate from 62.3% to 85.2% after 200 cycles at 4.5 V. Moreover, in a practical graphite||LCO pouch cell, the PAPDMS-modified LCO demonstrates superior long-term stability with 78.2% capacity retention after 500 cycles, dramatically outperforming pristine LCO electrodes (46.8%). This strategy presents a scalable approach to stabilizing high-voltage LCO in next-generation lithium-ion batteries.
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PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Jimin Qiu,Yuchen Ji,Wenfang Li,Yuhang Li,Wenguang Zhao,Yunxing Zuo,Weiyuan Huang,Chen Zhu,Mingjian Zhang,Guorui Zheng,Luyi Yang,Feng Pan,Zu-Wei Yin
Lithium cobalt oxide (LiCoO2) cathodes suffer serious structure instability when charged to high voltage (>4.5 V), including H1-3 phase transition, cobalt dissolution, and interfacial side reactions, which are closely related to the instability of surface lattice oxygen. Herein, an interfacial B–O complexing strategy was proposed to stabilize the surface lattice oxygen of LiCoO2 at 4.6 V, through the preferential coordination between derived products of the tris(pentafluorophenyl)borane electrolyte additive and LiCoO2. Combining a series of in situ and ex situ characterization methods with temporal and spatial resolution, it was revealed that the emergence of peroxy-like species (O22–) at high potentials is one of the origins of the instability of LiCoO2, which can be well inhibited thanks to interfacial B–O complexing. Thus, oxygen loss and interfacial side reactions can be drastically retarded, which consequently provides a more stable chemical environment for Co element, avoiding the dissolution and valence reduction of Co. Owing to the well-anchored Co and O elements, undesirable phase transition and local coordination structure change are suppressed, hence improving the capacity retention and rate performance of LiCoO2 at 4.6 V. This study provides an interfacial complexing strategy to stabilize the high-voltage LiCoO2 cathode.
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PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 42
·2304008
·
IF 19
Wen Zhang,Fangyuan Cheng,Meng Wang,Jia Xu,Yuyu Li,Shixiong Sun,Yue Xu,Liang Wang,Leimin Xu,Qing Li,Chun Fang,Yuhao Lu,Jiantao Han
Rapidly increasing demand for energy density in consumer electronics is eager for developing high-voltage LiCoO 2 (LCO). However, some great challenges such as severe phase transition and surface instability negate the cycle life of LCO operated at high-voltages (≥4.6 V). Herein, a chemical reconstruction strategy is proposed to form a collective surface of LCO through an interdiffusion reaction of MgHPO 4 ·3H 2 O (MP) so as to extend the cycle life of high-voltage LCO. The collective surface renders a three-layer configuration that demonstrates an amorphous Li 3 PO 4 outmost layer, a spinel-like layer beneath, and a Mg diffusion layer within LCO bulk. MP with relatively low hardness enables the uniform precoating via mechanical mixing, followed by a sintering process to undergo an interdiffusion reaction. Li 3 PO 4 is an intrinsic electrochemical stabilizer against interfacial side reactions. The spinel-like compounds build a high-voltage-stable surface against irreversible O 2 release. In addition, Mg diffuses into the bulk lattice to suppress irreversible phase transition during the deep delithiation of LCO. Therefore, such modified LCO with a collective surface exhibits ultralong life with capacity retention of 82% after 1000 cycles at 1 C within 3.0–4.6 V and stable operating at 4.7 V or elevated temperature (45 °C).
研究领域:
材料科学
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电化学
·
能源存储
·
无机化学
·
固态化学
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DOI
高影响因子
IONICS
·
2026
·
IF 3.4
Wu Keying,Tang Haiwen,Liu Yao,Wang Dan,Jiang Jinjin,Yu Liusi,Wang Sujun,Chen Lei,Tang Kai
LiCoO₂ (LCO) cathodes suffer from severe interfacial degradation, including cobalt dissolution, oxygen loss, and structural collapse, when cycled at high voltages (> 4.6 V), which limits their practical application. To address this issue, we propose a heterojunction engineering strategy via surface coating with lithium zirconium phosphate (Li₂Zr(PO₄)₂, LZP). The optimized LCO@LZP cathode delivers an ultrahigh initial discharge capacity of 178.1 mAh·g − 1 at 1 C (3.0–4.6 V) and retains 86.3% of its capacity after 200 cycles, significantly outperforming bare LCO (76.0%). It also exhibits enhanced rate capability (108.7 mAh·g − 1 at 10 C) and near-complete capacity recovery (99.7%) upon returning to 0.1 C. Mechanistic studies reveal that the LZP coating stabilizes lattice oxygen through robust Zr–O and P–O bonds, suppresses electrolyte decomposition to form a thin and inorganic-rich cathode electrolyte interphase (CEI), and enhances Li + diffusion kinetics (DLi + = 8.51 × 10 − 12 cm 2 ·s − 1 , 2.4 times higher than bare LCO). DFT calculations further confirm that the LCO/LZP heterojunction reduces oxygen charge compensation and creates an internal electric field that facilitates ion transport while inhibiting electron leakage. This work provides a scalable surface-modification strategy for developing high-energy-density LCO cathodes for next-generation lithium-ion batteries.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Xiaoyan Yu,Meng Li,Jun Ma,Yue Wang,Jingyi Qiu,Wenjie Meng,Zhenwei Zhu,Gaoping Cao,Yuehua Wen
Composite polymer electrolytes (CPEs) made of poly(ethylene oxide) (PEO) have potential applicability in future solid-state rechargeable Li-metal batteries (LMBs). However, the interfacial instability between high-voltage cathodes (HVC) and PEO-based CPEs currently limits their use in high-energy-density (HED) LMBs. In this study, an innovative interface engineering method is demonstrated to enhance interfacial stability by impregnating LiTFSI and LiDFOB dissolved in molten poly(ethylene glycol) dimethyl ether (PEGDME) in the cathode-contacting layer. The resulting dual-salt-containing polymer interphase displays high ionic conductivity, improved film-forming properties, and robustness. The interface-modified PEO-based CPEs have good interfacial adhesion with HVC. When charged to 4.3 V in the CPEs, the LiCoO2||Li cell delivers a superior rate capability at 60 °C, achieving stable cycling while retaining 87.2% of the initial capacity after 200 cycles at 60 °C and 86.6% after 460 cycles at 50 °C. This work provides a novel and viable approach to enhance the interface stability between PEO-based CPEs and high-voltage cathodes, advancing the development of safe LMBs with HED.
研究领域:
材料科学
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储能技术
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电化学
·
聚合物科学
·
锂离子电池
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DOI
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
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高影响因子
Science China-Materials
·
2022
·Vol. 66
·期 3
·903-912
·
IF 8.64
Zhong Wei,Zhang Ce,Li Siwu,Zhang Wei,Zeng Ziqi,Cheng Shijie,Xie Jia
Irreversible lithium loss in the initial cycles appreciably reduces the energy density of lithium-ion batteries. Prelithiation is an effective way to compensate for such lithium loss, but current methods suffer from either the instability or low capacity of prelithiation reagents. Lithium oxalate (Li 2 C 2 O 4 ) has shown great potential as a lithium-compensation material because of its high theoretical capacity (equivalent to lithium metal), low cost, and air stability. However, the practical applications of Li 2 C 2 O 4 are limited by its low electrochemical activity and high critical decomposition voltage. In this study, we performed the prelithiation of a low-voltage cathode by using Mo 2 C catalysis and nano-Li 2 C 2 O 4 . Results show that the Mo 2 C catalyst changes the electron cloud distribution around Li 2 C 2 O 4 and greatly reduces the activation energy, thereby significantly accelerating the lithium release from Li 2 C 2 O 4 . The nano-Li 2 C 2 O 4 prepared by freeze-drying shows accelerated ionic and electronic conduction as well as close contact with Mo 2 C. Benefiting from the synergistic effect, the decomposition potential of Li 2 C 2 O 4 is decreased by 0.5 V with an efficiency close to 100%. The LiCoO 2 ∥SiO full cell empowered with the nano-Li 2 C 2 O 4 /Mo 2 C prelithiation composite demonstrates 46.9% higher capacity than the control and thus has great potential for practical applications.
研究领域:
储能
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材料科学
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电化学
·
纳米技术
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Lianqi Zhao,Pu Yan,Tianying Liu,Xingzhi Wang,Zeyu Wang,Cong Wu,Wenda Bao,Haiyin Zhu,Yue Zhang,Jin Xie
High-voltage lithium cobalt oxide (LiCoO2) has the highest volumetric energy density among commercial cathode materials in lithium-ion batteries due to its high working voltage and compacted density. However, under high voltage (4.6 V), the capacity of LiCoO2 fades rapidly due to parasitic reactions of high-valent cobalt with the electrolyte and the loss of lattice oxygen at the interface. In this study, we report a temperature-driven anisotropic doping phenomenon of Mg2+ that results in surface-populated Mg2+ doping to the side of the (003) plane of LiCoO2. Mg2+ dopants enter the Li+ sites, lower the valence state of Co ions with less hybridization between the O 2p and Co 3d orbitals, promote the formation of surface Li+/Co2+ anti-sites, and suppress lattice oxygen loss on the surface. As a result, the modified LiCoO2 demonstrates excellent cycling performance under 4.6 V, reaching an energy density of 911.2 Wh/kg at 0.1C and retaining 92.7% (184.3 mAh g–1) of its capacity after 100 cycles at 1C. Our results highlight a promising avenue for enhancing the electrochemical performance of LiCoO2 by anisotropic surface doping with Mg2+.
研究领域:
材料科学
·
电化学
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PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2020
·
IF 3.83
Jun Ping,Sajid Rauf,Zuhra Tayyab,Ruilong Wang,Haibo Xiao,Lingfang Xu,Shiheng Liang,Qiuan Huang,Changping Yang
Lithium cobalt oxide (LCO) with layered crystal structure suffers the structural proton intercalation in aqueous electrolytes of low pH values, little information is available about the effect of microstructure change on the cycling stability of LCO in response to the proton intercalation. In this work, electrochemical properties of three kinds of LCO spheres with different microstructures are studied in neutral aqueous 0.5 M Li 2 SO 4 solution. The investigated materials were obtained by calcining the spherical LCO precursors at various temperatures, which were synthesized via a modified solid phase method for lithiation of spherical Co 3 O 4 . Structure and morphology of materials were characterized by X-ray diffraction (XRD) and field emission scanning electron microscope (FE-SEM). The spherical LCO prepared at lower temperature shows more superior electrochemical stability. Herein, the resistance of spherical LCO with a particular microstructure to the electrode degradation for the proton intercalation can be measured by the frequency of occurrences of greater-than-100% coulombic efficiencies during cycling. Meanwhile, the capability of retaining the capacity contribution from the order-to-disorder transformation of lithium ions on the hexagonal lattice of host site after the first-order phase transition was proposed to compare and investigate the cyclability of the three kinds of spherical LCO with different microstructures.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Zhou Xing,Chang Chia-Yu,Yu Dongfang,Zhang Kai,Li Zhi,Jiang Shi-Kai,Zhu Yizhou,Xia Yongyao,Hwang Bing Joe,Wang Yonggang
The application of high-voltage positive electrode materials in sulfide all-solid-state lithium batteries is hindered by the limited oxidation potential of sulfide-based solid-state electrolytes (SSEs). Consequently, surface coating on positive electrode materials is widely applied to alleviate detrimental interfacial reactions. However, most coating layers also react with sulfide-based SSEs, generating electronic conductors and causing gradual interface degradation and capacity fading. To address this, we propose a Li 2 ZrF 6 coating layer on LiCoO 2 , which exhibits minimal reaction with SSEs, and its decomposition products are electron-conductive-free. Furthermore, this coating layer also efficiently mitigates the layered-to-spinel/rock-salt surface structural transformation in LiCoO 2 . As a result, the In-Li|Li 6 PS 5 Cl | Li 2 ZrF 6 -LiCoO 2 all-solid-state cell demonstrates an initial areal capacity of 5.2 mAh cm −2 and a capacity retention of 80.5% after 1500 cycles at 70 mA/g with high LiCoO 2 areal mass loading (30.19 mg cm −2 ) and a cut-off voltage of 3.9 V (corresponding to potential of 4.5 V versus Li + /Li), at 25 °C.
研究领域:
材料科学
·
能源存储技术
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DOI
PubMed
高影响因子
Nature Communications
·
2026
·Vol. 17
·期 1
·41
·
IF 15.7
Liu Ganxiong,Nie Quan,Wan Wang,Yang Fangzhou,Yang Zhiqi,Qu Ge,Guo Lingling,Chen Jitao,Wei Xuezhe,Huang Yunhui,Wang Chao
Battery recycling is essential to mitigate resource depletion and improve environmental sustainability. However, conventional metallurgical and direct regeneration methods involve trade-offs among energy input, environmental impact, and feedstock adaptability. Here we report a universal upcycling method that converts spent LiCoO 2 into Li 6 CoO 4 within 10 seconds via flash Joule heating, achieving complete lithium and cobalt recovery regardless of degradation state. The resulting Li 6 CoO 4 serves as a high-capacity sacrificial additive to offset active lithium loss. To overcome its inherent air sensitivity and oxygen release during delithiation, a conformal sulfur coating was applied to stabilize surface chemistry and redirect oxygen evolution into sulfate formation. This sulfur-mediated mechanism effectively suppresses gas generation and parasitic side reactions, enabling non-destructive lithium replenishment. When integrated into graphite | |LiFePO 4 pouch cells, the stabilized Li 6 CoO 4 achieves 91.4% capacity retention over 1400 cycles at a current density of 80 mA g −1 . Comparative life-cycle and techno-economic analyses reveal clear reductions in energy consumption and CO 2 emissions, along with improved economic returns. This work provides a scalable route that bridges positive electrode waste recovery with high-performance lithium supply, advancing closed-loop battery systems for sustainable energy storage.
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高影响因子
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