ACS Applied Energy Materials
·
2020
·
IF 4.473
Wen Liu,Xifei Li,Youchen Hao,Hirbod Maleki Kheimeh Sari,Jian Qin,Wei Xiao,Xiujuan Wang,Huijuan Yang,Wenbin Li,Liang Kou,Zhanyuan Tian,Le Shao,Cheng Zhang,Jiujun Zhang
LiNi0.8Co0.1Mn0.1O2 (NCM) is a highly prospective cathode material for high energy density Li-ion batteries (LIBs). Nevertheless, poor cycling performance and rate capability at high cutoff voltages have dramatically blocked its further commercialization. In this study, an ionic conductive interface has been demonstrated to enhance the NCM electrochemical property at the high cutoff voltage of 4.5 V on account of the existence of a Li-ion conductor of Li2SnO3. In comparison to SnO2, Li2SnO3 causes a smoother Li-ion diffusion at the engineered interfaces, lower polarization, slower capacity drop, and voltage fading as well as better H2/H3 reversibility upon cycling. Importantly, it is confirmed that excellent diffusion is beneficial to preservation of reversible phase transition and reduction of polarization, which are directly relative to the superior cyclability and rate capability. This work reveals that building an excellent ionic diffusion interface is feasible for Ni-rich cathodes with simultaneous high capacity and stable cyclability.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
ENERGY & FUELS
·
2026
·Vol. 40
·期 29
·15968-15978
·
IF 6
Li Qingbin,Li Zhenguo,Li Kaixiang,Tian Runfeng,Liu Xianhua,Zou Yuxiao,Zhao Pengcheng,Lu Yiren
The
rapid growth of Li-ion battery consumption has led to an increasing
number of spent batteries, posing serious challenges to resource sustainability
and environmental protection. This study develops a low-carbon, W-doping-assisted
direct regeneration strategy for spent LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) cathode materials, aiming
to realize simultaneous lattice restoration, microstructural reconstruction,
and interfacial stabilization. The regeneration process involves hydrothermal
relithiation combined with W incorporation and high-temperature annealing.
Comprehensive characterizations, including XRD, XPS, SEM, HRTEM, EPR,
and electrochemical analyses, reveal that the proposed method effectively
reconstructs the layered R 3 ¯ m structure and recovers long-range order while eliminating impurity
phases. W incorporation enhances structural integrity by forming robust
W–O bonds, suppressing oxygen vacancy formation, mitigating
Li/Ni cation mixing, and reducing microcrack propagation. Furthermore,
the regeneration process restores the high oxidation states of transition
metals (Ni 3+ , Co 3+ , Mn 4+ ), thereby
stabilizing the lattice and improving charge-transfer kinetics. The
regenerated cathode exhibits a high initial discharge capacity of
approximately 163 mA·h·g –1 , reduced polarization,
and excellent cycling stability comparable to or surpassing that of
fresh NCM523. Overall, this work demonstrates that W-doping-assisted
direct regeneration provides an effective and sustainable pathway
for multiscale structural recovery of spent NCM cathodes, promoting
high-value utilization in circular battery recycling.
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高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 167
·期 16
·160557
·
IF 4.316
Guange Wang,Tong Wu,Borui Liu,Shanshan Gong,Qing Huang,Yuefeng Su,Feng Wu,Ryan M. Kelly
Considering that lithium-ion battery (LIB) is still an indispensable and important component of energy storage materials, the sustainable post-processing of spent LIBs in labs or enterprises becomes a tricky problem. Herein, a novel scheme is proposed to dissert the recycling of the spent LIBs. The LIB is recycled into Li(Ni0.9Co0.05Mn0.05)O2 (NCM90) cathode material with high specific capacity by introducing an innovative hydrometallurgy-coprecipitation treatment method. The spent LiCoO2 (LCO) cathode material is firstly leached by sulfuric acid, and the leachate is gradient used as the raw materials to resynthesize high-nickel NCM material by adjusting the leachate dosage to about 50%. Interestingly, when the dosage exceeds 50%, the crystal structure aggravates, and Li+/Ni2+ mixing improves. The specific capacity of regenerated battery is 181.4 mAh g−1 at 0.5 C (1 C = 200 mAh g−1) and the capacity retention achieves 93.2% after 100 cycles. The reasons can be attributed to the cation mixing and crystal strucure and the small amount of Al doping. In conclusion, this combined method recycling of LIBs has huge potential value for environment protection and production.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qing Zhang,Naiqian Sun,Weiguang Lv,Yue Wang,Zhi Sun
In the recycling of spent lithium-ion batteries, pretreatment is an essential step to separate cathode materials from aluminum current collectors. However, it is typically energy-intensive, with high chemicals consumption and metal loss. In this research, we demonstrate a sustainable and straightforward strategy to acheive stepwise recovery of Li and transition metals without pretreatment step. In a mildly acidic hydrothermal environment, the interaction between aluminum current collectors and cathode materials results in the formation of AlO(OH) interlayers, which preserves the sandwich-like structure of the leaching residue while lithium can be selectively recovered. In the leaching residue, the cathode materials are transformed into a low-valence transition metal hydroxides, which are more easily to be reacted than the passivated aluminum foil and other impure compounds (e.g. binder, TiO 2 and other oxide additives etc.) under mild acidic solutions. As a result, the transition elements i.e. Ni, Co, Mn can be selectively recovered. Therefore, 90.0 % of Li and more than 95.0 % of transition metals are successfully recycled, with Al and other impure compounds being conserved in the leaching residue. This research proves it is possible to achieve selective metal recovery while skiping the pretreatment step and offers new perspectives on the recycling of valuable metals from spent lithium-ion batteries.
研究领域:
材料科学
·
环境工程
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DOI
高影响因子
Surfaces and Interfaces
·
2025
·
IF 6.3
Mihong Cao,Lucheng Li,Wenfeng Yuan,Jun Chen
In order to solve the problems of insufficient adsorption electrolyte capacity and small specific surface area caused by the smooth surface and few pores of Super P spherical conductive particles, this work uses concentrated sulfuric acid (H 2 SO 4 ) for surface etching of Super P conductive particles to explore the influence of different etching time on the micromorphology of SP conductive agent and the behaviors of LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM-523) batteries. After etched by concentrated H 2 SO 4 , the surface of SP conductive agent changes from “capillary” structure to fluffy “plush” structure, effectively improving the conductivity specific surface area of the conductive agent particles. Compared with the pristne SP-0H conductive agent, the batteries using 1.5% of concentrated H 2 SO 4 etched SP-1H, SP-2H and SP-20H conductive agent have smaller EIS impedance value, larger area of CV curves, and smaller potential difference of the redox peaks. As a result, the initial charging/discharging capacities of SP-1H, SP-2H and SP-20H conductive batteries were 178.7/183.0, 187.6/183.9, 178.9/180.8 mAh/g with corresponding ICE of 102.4%, 98.0% and 101.1% respectively, which were much higher than the pristine SP-0H conductive battery (182.0/173.7 mAh/g with ICE of 95.4%). In addition, the SP-1H, SP-2H and SP-20H batteries also show significantly improved cycle performance and rate cycle capabilities, showing more superior comprehensive behaviors, which can provide a new modification insights for the exploration of new conductive agent in NCM-523 of high-performance lithium ion batteries.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Materials Today
·
2022
·
IF 26.943
Yun Liu,Qi Wang,Lai Chen,Zhiming Xiao,Xinming Fan,Shuailing Ma,Lei Ming,Akhil Tayal,Bao Zhang,Feng Wu,Xing Ou
Nickel-rich layered LiNi x Co y Mn 1- x - y O 2 (NCM, x ≥ 0.83) is considered as a promising cathode material for lithium-ion batteries (LIBs), owing to its satisfying specific energy. However, the undesired phase transformation from layered into rock-salt at the NCM surface will easily induce Li concentration gradient during cycling, which hinders the Li-ions diffusion and leads to the gradual accumulation of inner stress with the appearance of microcracks. Herein, we propose a surficial engineering strategy to promote the Li-ions transmission for single-crystalline LiNi 0.83 Co 0.11 Mn 0.06 O 2 (SCNCM) via Li 1.3 In 0.3 Ti 1.7 (PO 4 ) 3 (LITP) modification. It is noted that, as the fast Li-ion conductor, LITP can accelerate the Li-ions diffusion and alleviate the electrode–electrolyte side reaction simultaneously. More importantly, LITP can serve as the Li-ions regulator, ensuring the homogeneous distribution of Li-ions and minimizing the concentration difference at SCNCM surface. It can relieve the stress induced by the inconsistent Li-ions dispersion, which effectively decreases the degree of structural disordering and lattice mismatch at surface, eventually maintaining the high structure integrity during long-term cycling. As anticipated, even under the harsh testing conditions, the LITP modified SCNCM still can achieve a satisfied reversible capacity of 196.4 mAh g −1 under potential range of 2.75–4.6 V after 200 cycles at 25 °C in coin-type half-cells. Furthermore, it provides an extraordinary capacity retention of 88% in 2.75–4.3 V after 400 cycles at high temperature of 45 °C in pouch-type full-battery.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Lijie Zhai,Mengting Lv,Mengmeng Cong,Tao Lin,Nan Meng,Fang Lian,Huiping Shao
The LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM) electrodes are successfully prepared by 3D gel printing (3DGP) technique in this study. The results show that when the slurry with 45 % solid content was squeezed out of the needle, the viscosity of the printing slurry was 1.54 Pa s at the shear rate of 660 s −1 , which shows that the printing slurries are suitable for 3DGP. At the same time, when the inner diameter of the printing needle is 0.25 mm, the air pressure is 0.40 MPa and the printing speed is 4.60 mm s −1 , the structure of printing electrode is complete. The electrochemical measurement results show the printed NCM electrode with 231 μm printing line spacing has a higher capacity of 169.80 mAh g −1 at 4C, a specific capacity of 103.9 mAh g −1 at 1C after 500 cycles and an energy density of 232 Wh kg −1 , which shows that the high specific capacity and good cycling stability exhibited by NCM electrodes fabricated by 3DGP.
研究领域:
材料科学
·
电化学
·
能源存储
·
增材制造
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DOI
高影响因子
Small
·
2025
·Vol. 21
·期 24
·2503589
·
IF 12.1
Qiaoling Qiu,Jiafeng Ruan,Wei Zhou,Wenqiang Hu,Wei Wu,Jichao Zhang,Fang Fang,Dalin Sun,Jiahe Zang,Yun Song
A small amount of Mg 2+ doping can show a significant effect on the surface protection and structural stability of the nickel-rich layered oxide cathode, but the traditional doping process involves completely changing the initial raw material proportions with subsequent trial and error adjustments. Herein, a concept of Mg 2+ release film is proposed, in which Mg 2+ can easily permeate into various layered oxide cathodes during cycling. Meanwhile, to realize this concept, MgV 2 O 4 with mobile Mg 2+ in the structures and then fabricated a self-supporting MgV 2 O 4 membrane are synthesized. As a protective layer for cathode, the MgV 2 O 4 membrane release Mg 2+ in situ during the electrochemical process, providing structural reinforcement to the cathode surface as a “pillar” within the lattice. Thanks to the MgV 2 O 4 membrane, the cycle life of LiNi o.8 Co 0.1 Mn 0.1 O 2 (NCM811) coupled with the MgV 2 O 4 interlayer at 1.0 C is increased by 1.9 times compared to bare NCM811. Furthermore, this novel Mg 2+ releasing film demonstrates excellent versatility, enabling other nickel-based layered oxide to achieve a high-capacity retention of 86.4% after 800 cycles at 1.0 C. This approach provides scalable cathode protection and repair strategies for commercially viable batteries.
研究领域:
材料科学
·
电化学
·
储能
·
电池技术
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Long Ye,Xinyou He,Yao Shi,Zhiming Xiao,Wei Wang,Lei Cheng,Xinming Fan,Bao Zhang,Xing Ou
The instability in the structural integrity caused by interfacial issues is commonly regarded as the primary drawback of Ni-rich layered cathode materials (LiNi x Co y Mn 1-x-y O 2 , where x ≥ 0.8), which must be addressed before their commercial application. Herein, a novel multiple-function surface modification strategy is proposed based on the single crystal structure to in-situ achieve the construction of a coating layer and surface doping with Ce element to enhance the structural stability of the LiNi 0.88 Co 0.09 Mn 0.03 O 2 (NCM). Notably, the introduction of Ce-O bonding adjusts the local oxygen coordination to achieve a more stabilized structure of the oxygen framework, which inhibits the evolution of lattice oxygen and enhances conductivity. Additionally, by benefiting from the in-situ synthesized coating layer of Li x CeO 2 , the occurrence of side reactions on the surface is effectively alleviated, resulting in a reduction in electrode polarization. Combined with comprehensive electrochemical tests, it is confirmed that the improved electrochemical performance originates from the reduction of the detrimental H2-H3 phase transition and enhanced conductivity. As expected, the modified material with 1 wt% content of Ce (NCM@Ce) exhibits a high initial discharge capacity of 196.3 mAh g −1 with a capacity retention of 79.7 % after 200 cycles, and its energy density reaches 574.3 Wh kg −1 after 200 cycles.
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Pengcheng Zhao,Yao Li,Xiaoyu Wang,Xiaoman Liu,Pei Gao,Peng Guo,Xiaoxiang Wang,Chunfei Wu,Boxiong Shen
With the large-scale application of power batteries, a large number of spent lithium-ion batteries (LIBs) will be formed in recent years. The improper disposal of spent LIBs will pose significant environmental pollution. LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM), as a typical type of LIBs cathodes material, are widely used and can be highly recycled. However, the existing hydrometallurgical and pyrometallurgical recycling processes consume large amounts of energy and introduce serious secondary pollution. This work presents a simple straightforward direct regeneration process that uses urea solvothermal treatment followed by calcination to obtain urea-regenerated spent NCM (UR-S-NCM). Surprisingly, the specific capacity of the regenerated NCM of UR-S-NCM recovers completely and reaches 166 mAh/g, higher than that of fresh NCM (F-NCM) at 156 mAh/g. After 100 charge/discharge cycles, the specific capacity of UR-S-NCM is 37 % higher than that of F-NCM at the same condition. Additionally, the CO 2 emissions per kilogram of the regenerated UR-S-NCM are only 1.79 kg, about 31 % of pyrometallurgy and 48 % of hydrometallurgy, respectively. The surface smoothness, grain boundaries and layered structure of UR-S-NCM are recovered from S-NCM to the same situation of F-NCM. Smooth surface facilitates Li + migration into and out of UR-S-NCM, grain boundaries reduction diminishes electrolyte corrosion, and the layered structure accommodates more Li + compared to the spinel structure of S-NCM. This work provides an eco-friendly direct regeneration process and offers a new insight for LIBs regeneration.
研究领域:
材料科学
·
环境科学
·
能源科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Yangfan Zhou,Ziyi Hu,Yuhui Huang,Yongjun Wu,Zijian Hong
Solution wash is a key procedure in the recycling of cathode materials for lithium-ion batteries. It is well-known that Ni-rich ternary cathode material LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM-811) is sensitive to water, triggering the Li + /H + exchange and increasing the cation disorder, which ultimately leads to a large capacity loss during the battery cycling. In this study, we investigated the structural/surface chemical stability as well as the capacity loss for NCM-811 ternary cathodes after washing in five different environmentally friendly and commercially available solutions (i.e., ethanol, methanol, sodium chloride aqueous solution, sodium hydroxide aqueous solution, and deionized water). It is discovered that the capacity decay rate during cycling is closely related to the Li + ion loss after solution wash, the more the Li + ion loss, the quicker the capacity decay during cycling. Among all the solution-washed samples, ethanol-washed samples show minimal Li + ion loss and the best capacity retention. Where the Li + ion loss is only 2%, and the specific capacity after 200 cycles is 2.6 times higher as compared to the water-washed counterparts. This study paves the way towards the practical applications of ethanol in the commercial recycling of NCM-based cathodes.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Coatings
·
2021
·Vol. 11
·期 8
·932
·
IF 2.881
Chen Xu,Siqi Guan,Lixiang Li,Chengguo Sun,Baigang An,Xin Geng
The content of ammonia coordination agent in initial aqueous solution is one of important factors which greatly influences the morphologies and electrochemical performances of layered LiNi6Mn2Co2O2(NCM622). The spherical morphologies, contributing to higher specific capacity of NCM622, ascribe to the same precipitation rate of transition metal ions (Ni2+, Co2+, Mn2+) during co-precipitation. Hence, the effects of different amounts of ammonia in initial solution on the hydroxide equilibrium constant and properties of NCM622 were discussed. With the ammonia content of 70 mL, the spherical morphology with more perfect layered structure and higher discharge capacity are obtained. The necessity of ammonia content in initial solution are also demonstrated from electrochemical performances of NCM622, such as the initial discharge capacity of 199.8 mAh g−1at 0.1 C, the specific capacity of 150.0 mAh g−1after 100th cycles, and the capacity retention rate of 89.6% at 3 C. If other metal ions are anticipated to be chemically doped with NCM622, the hydroxide equilibrium constant and precipitation rate need to be considered.Keywords:lithium ion batteries;hydroxide co-precipitation method;NCM ternary precursor;electrochemical performance
研究领域:
材料科学
·
电化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）