ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Kang Liu,Zibo Xu,Mengmeng Wang,Daniel S. Alessi,Yuanzhi Tang,Daniel C. W. Tsang
Resource recovery from retired electric vehicle lithium-ion batteries (LIBs) is a key to sustainable supply of technology-critical metals. However, the mainstream pyrometallurgical recycling approach requires high temperature and high energy consumption. Our study proposes a novel mechanochemical processing combined with hydrogen (H2) reduction strategy to accelerate the breakdown of ternary nickel cobalt manganese oxide (NCM) cathode materials at a significantly lower temperature (450 °C). Particle refinement, material amorphization, and internal energy storage are considered critical success factors for the accelerated decomposition of NCM cathode materials. In our proposed approach, NCM cathode materials can develop active sites with carbon defects (Cv) and oxygen vacancies (Ov), which improve the reduction and breakdown of H2. The adsorbed H2 on the surface of NCM decomposes into H* and combines with oxygen to form OH species, which can be facilitated by Ov via the enhanced charge transfer. The introduced Cv can enhance H2 cracking and generate *C–H species to promote the thermal decomposition of NCM. The presence of defects proves to foster the preferential reduction of Mn(IV) by H2, leading to a lower activation energy for the NCM decomposition (from 139 to 110 kJ/mol) with less H2 consumption. Life cycle assessment suggests a reduction of 4.42 kg CO2 eq for the recycling of every 1.0 kg of retired batteries. This study can promote material circularity and minimize the environmental burden of mining technology-critical metals for a low-carbon transition.
研究领域:
材料科学
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环境科学
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能源工程
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高影响因子
Journal of Materials Research and Technology-JMR&T
·
2026
·
IF 7.3
Xiangli Wen,Mingkun Bi,Lvzhou Li,Jianning Ding
SUS304 steel is widely employed as the core component material in battery slurry homogenization equipment. However, due to its insufficient hardness and poor resistance to plastic deformation, severe abrasive wear and oxidative corrosive wear tend to occur during the homogenization process, which further deteriorates the battery performance. In this work, targeting the special medium of battery slurry, three potential screw materials for application in battery slurry systems were selected: 40Cr alloy steel, 440C martensitic stainless steel, and GCr15 bearing steel. The friction behavior laws and wear resistance mechanisms of these materials in lithium iron phosphate (LFP) and lithium nickel cobalt manganese oxide (NCM) slurries were systematically investigated using an atmosphere friction and wear tester. The results demonstrate that all three materials exhibit superior wear resistance compared to SUS304. Among them, the chromium-rich hard phase in 440C delivers excellent anti-wear properties, making it suitable for medium-to-high speed homogenization, especially with outstanding performance in LFP slurry. GCr15 possesses a uniform and stable phase structure composed of carbides and martensite, resulting in broader adaptability to various working conditions. It maintains an extremely low wear rate ( δ ) with minimal fluctuation in both slurries, and the reduction in δ exceeds 90% under high-speed and high-load conditions, revealing the optimal comprehensive performance. This work provides important theoretical basis and experimental support for material selection of key components in battery homogenization equipment, and is of positive significance for improving equipment reliability and ensuring the quality of battery slurry.
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WASTE MANAGEMENT
·
2026
·
IF 7.1
Maoting Yu,Chengping Li,Ailin Xu,Bo Li,Yushu Wu,Boyue Dong,Zhaohui Zheng,Jinsong Wang,Yingjie Zhang,Peng Dong,Chongjun Bao,Zhengfu Zhang
The rapid expansion of electric vehicles has driven a surge in end-of-life lithium-ion batteries (LIBs). Conventional hydrometallurgical recycling, dependent on strong inorganic acids and chloride-containing reagents, induces severe secondary pollution and equipment corrosion. Although deep eutectic solvents (DESs) are extensively explored as green alternatives, mainstream chloride salt-acid systems persistently risk chlorine contamination, necessitating inherently safe chloride-free alternatives. This study developed a novel chloride-free DES with excellent recyclability using trimethylglycine (TMG) and glycolic acid (GA). Response surface methodology (RSM) optimization yielded optimal leaching conditions: 1.95 h, TMG:GA molar ratio of 1:3.2, S/L of 20 g/L, and 99 °C. Under these conditions, unprecedented leaching efficiencies (>99%) for Li, Ni, Co, and Mn from spent LiNi 1/3 Co 1/3 Mn 1/3 O 2 (NCM111) were achieved, with demonstrated universality across multiple cathode configurations (>94%). The kinetic study showed that the leaching process is governed by surface chemical reaction, with activation energies of 33.19/42.61/40.50/37.38 kJ mol -1 for Li/Ni/Co/Mn. Density functional theory (DFT) calculations unveiled that the DES disrupts metal–oxygen (M−O) bonds via a synergistic reductive-chelation mechanism, where binding energies followed Mn > Co > Ni. This work offers a promising approach for recycling spent batteries with its environmental friendliness, high efficiency, broad applicability, and in-depth mechanism.
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Materials Horizons
·
2025
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IF 10.7
Yuzhang Xiao,Zhi Gao,Weihao Lin,Guangyao Yang,Sikai Peng,Yihong Tong,Weiliang Peng,Bin Yuan,Renzong Hu,Wei Min Huang
In the recycling process of spent lithium-ion batteries (SLIBs), rapid and effective separation of cathode material and current collector aluminium (Al) foil is a significant and difficult step. However, traditional separation methods have some drawbacks including high energy consumption, expensive and toxicity. In this study, we select oxalic acid (OA), a green and low-cost simple organic acid, as the separating agent. Within 10 minutes oxalic acid treatment, above 99% of the nickel-manganese-cobalt (NCM) cathode materials are separated from current collector Al foil. The mechanism analysis shows that the reaction of oxalic acid with the surface of Al foil can destroy the connection between Al foil and adhesive, while the oxalate protective layer formed on the surface of NCM cathode material prevent further corrosion of NCM cathode material, maintaining a good structural integrity. This green and efficient separation method provides an economical and viable solution for SLIB regeneration or upcycling.
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ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Zelin Li,Xinping Chen,Wenting Li,Jie Li,Yujuan Zhang,Lisi Lu,Chun Zhan,Xinping Qiu
Lithium metal batteries (LMBs) combined with a high-voltage nickel-rich cathode show great potential in meeting the growing need for high energy density. The lack of advanced electrolytes has been a major obstacle in the commercialization of high-voltage lithium metal batteries (LMBs), as these electrolytes need to effectively support both a stable lithium metal anode (LMA) and a high-voltage cathode (>4 V vs Li+/Li). In this work, by extending the two terminal methyl groups in DIGDME and TEGDME to n-butyl groups, we design a new weakly solvating electrolyte (2 M LIFSI+TEGDBE) that enables the stable cycling of NMC83 (LiNi0.83Co0.12Mn0.05O2) cathodes. The NMC83 cell exhibits a high and stable Coulombic efficiency (CE) of over 99%, as well as capacity retention of approximately 99.8% after 100 cycles at 0.3 C. X-ray photoelectron spectroscopy analysis (XPS) and high-resolution transmission electron microscope (HRTEM) images revealed that the anion species decomposed first, resulting in the formation of a cathode–electrolyte interface (CEI) film predominantly consisting of decomposition products from the anions on the positive electrode surface. This work links the functional group of solvents with the solvation structure and electrochemical performance of ether-based electrolytes, providing a distinctive sight to design advanced electrolytes for high-energy-density LMBs.
研究领域:
材料科学
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电化学
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高影响因子
LANGMUIR
·
2023
·
IF 3.9
Shengde Dong,Fang Liu,Yue Leng,Yanxia Sun,Chunxi Hai,Xianfei Chen,Yuan Zhou
Ni-rich cathode materials show promise for use in lithium-ion batteries. However, a significant obstacle to their widespread adoption is the structural damage caused by microcracks. This research paper presents the synthesis of Ni-rich cathode materials, including LiNi0.8Co0.1Mn0.1O2 (referred to as NCM) and Li(Ni0.8Co0.1Mn0.1)0.98Al0.02O2 (referred to as NCMA), achieved through the high-temperature solid-phase method. Electrochemical (EC) testing results reveal the impressive EC performance of NCMA. NCMA exhibited a discharge capacity of 141.6 mAh g–1 and maintained a cycle retention rate of up to 74.92% after 300 cycles at a 1 C rate. In contrast, the NCM had a discharge capacity of 109.7 mAh g–1 and a cycle retention rate of 61.22%. Atomic force microscopy showed that the Derjaguin−Muller−Toporov (DMT) modulus value of NCMA exceeded that of NCM, signifying a greater mechanical strength of NCMA. Density functional theory calculations demonstrated that the addition of aluminum during the delithiation process led to the mitigation of anisotropic lattice changes and the stabilization of the NCMA structure. This improvement was attributed to the relatively stronger Al–O bonds compared to the Ni(Co, Mn)–O bonds, which reduced the formation of microcracks by enhancing NCMA’s mechanical strength.
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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高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2026
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IF 7.1
Wen-bo Lou,Yi-dan Zheng,Shu-han Zhang,Dong-yan Liu
The carbon thermal reduction process is considered an industrially promising method for spent ternary cathode materials. It’s comprehensive studies to address the reduction thermodynamics, phase transition, and kinetic behaviours of actual Al-containing ternary materials has received increasing attention. In this study, based on thermodynamic evaluation, under ideal conditions, both C and Al are suitable reducing agents. And the reduction difficulty is Mn > Co > Ni from thermodynamic and experimental analysis. The predicted products are mainly Ni, Co, CoO, NiO, MnO, Li 2 CO 3 , and Li-Al compounds. Further, phase transition analysis indicates that it is feasible to reduce the material while simultaneously suppressing Li-Al bonding, with composition of Ni or Co, Li 2 CO 3 , and MnO, by controlling the conditions of 700 °C for 2 h with 15% carbon. According to thermogravimetric analysis, this process can be roughly divided into three stages, including evaporation, decomposition and reduction, respectively. Finally, the results of kinetics analysis combining the Coats-Redfern and KAS/FWO models indicates that the corresponding activation energy increases from 13.46 kJ/mol to 481.53 kJ/mol across the reaction stages. This study may provide theoretical foundations for practical recycling of Al-containing battery materials, and demonstrate the broad prospects of the carbon thermal reduction process for industrial application.
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SOLID STATE IONICS
·
2019
·
IF 2.886
Songyi Han,Hong Zhang,Chaojun Fan,Weizhen Fan,Le Yu
Layered structure LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM) cathode has been considered as a higher energy density candidate, but the problems of high voltage cycling resistance hinders its further application. Herein, we report a Nitrile (-CN) group 1,4-Dicyanobutane (ADN) as a film forming additive. Linear sweep voltammetry (LSV) tests have shown that EC/EMC based electrolytes with ADN have higher oxidation potentials (>6.2 V vs. Li/Li + ). The LiNi 0.5 Co 0.2 Mn 0.3 O 2 /graphite full cells containing 0.5 wt% ADN showed significant high voltage cycling performance with a capacity retention of 85.2%, while the blank electrolyte after 120 high voltage cycles was 67.96%. This is attributed to the protective effect of SEI film prevents the further decomposition of electrolyte and transition metal ion dissolution, thus stabilizes the electrode-electrolyte interface. Scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS) results also demonstrate less unwanted lithium compounds absorbed on the ADN-contained cathode corresponding to fewer side reaction.
研究领域:
电化学
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材料科学
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能源存储
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电池技术
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电极-电解质界面
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Zhijie Bi,Tengfei Wang,Xiaotong Chang,Mengyang Jia,Xiangxin Guo
The garnet Li 7 La 3 Zr 2 O 12 solid electrolyte presents promising potential in application of solid-state lithium batteries because of its high ionic conductivity and stability. However, the critical interfacial issues between cathodes and garnet electrolytes severely restrict capacity and cycling stability of solid batteries. In this work, the partially cyclized polyacrylonitrile (cPAN) nanolayer is coated on high-voltage LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM) cathode particles enabling interface-friendly solid-state garnet batteries. Through controlling cyclized temperature and time, the cyclized part of polyacrylonitrile equipped with delocalized sp 2 π bond presents good capability for electronic transfer, while the residual part not involved in cyclization leaves the coating with certain feature for ionic transfer. In this way, such hybrid-conductivity coating facilitates the transport of both ions and electrons inside the cathode. In addition, the moderate cyclization condition retains the elasticity of polymers, contributing to protection of NCM cathode and suppression of side reactions at NCM/garnet interface during cycling. Therefore, the resultant solid NCM/garnet/Li cell based on the proposed interface engineering strategy delivers a discharge capacity of 176 mAh g −1 with a capacity retention of 82.4 % after 400 cycles. This work puts forwards an attractive strategy to modulate the cathodic interfaces toward solid-state garnet batteries via introducing partially cyclized polyacrylonitrile protective layer with hybrid conductivity.
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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固态电池技术
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 23
·2113068
·
IF 19.924
Xufeng Wang,Yajie Song,Xin Jiang,Qingsong Liu,Jidong Dong,Jian Wang,Xin Zhou,Bing Li,Geping Yin,Zaixing Jiang,Jiajun Wang
The complicated interfacial problems of poly(ethylene oxide) (PEO)-based solid polymer electrolytes (SPEs) at high voltages severely hinder its practical applications for high-energy-density all-solid-state lithium batteries (ASSLBs). Herein, the failure mechanisms of ASSLBs with LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM)-PEO are studied. It is found that the ASSLBs after charge generates a sharp drop of 0.62 V at the cut-off voltage of 4.30 V, and induce a high interfacial resistance due to forming an uneven thick cathode electrolyte interface on the NCM surface, as well as cause the destruction of NCM surface structure during storage, leading to serious performance degradation. Constructing the interfacial nanolayer with aromatic polyamide (APA) on the surface of NCM active particles (NCM@APA) can mitigate interfacial side reactions between NCM and SPE. Robust interfacial nanolayers not only effectively protect the crystal structure of NCM but also provide a steady interfacial environment for Li + diffusion kinetics. Accordingly, NCM@APA||SPE||Li ASSLBs exhibit an acceptable voltage drop of 0.27 V after 10 days storage and a substantially improved electrochemical performance with an average coulombic efficiency of 99.1% and capacity retention of 76.7% at 30 mA g −1 after 80 cycles.
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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高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
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IF 6.9
Jun Wang,Le Wang,Jiuyun Zhang,Zhixuan Wang,Yitao Liu,Wei Cai,Bin Fei,Renming Pan,Xia Zhou
The explosion characteristics of gases generated from the overcharged thermal runaway (TR) process of NCM pouch cell were investigated. Specially, the gases mainly include H 2 , CH 4 , C 2 H 4 , C 2 H 6 , C 3 H 6 , and CO, and its maximum explosion pressure (MEP) concentration is 25% (volume ratio). The lower explosion limit of TR gas is 11.15%, and the upper explosion limit is 36.875%. To reduce the risk of an explosion from the TR gas, a unique aerosol explosion suppression agent (ASA) was prepared using simple three-component raw materials and a freeze-drying process. For the TR gas explosion at MEP concentration, the ASA-0.3 g can decrease MEP by 74.64% and maximum explosion pressure rate (MPR) by 97.67%. The ASA-0.5 g can completely inhibit the explosion. The mixed gas was 5.3 L, so the explosion suppression concentration of ASA is 0.095 g·L -1 . It is found that ASA consists of a gas mixture of N 2 and CO 2 and solid reactive particle (SRP). The anhydrous SRP contains 33% nanoscale KHCO 3 particles with a particle size mainly range of 0.1–1 μm. And the D90 of SRP is about 0.63 μm. The minimum extinguishing concentration of ASA is from 30 to 40 g·m -3 . Additionally, typical radiation spectra of potassium ions are found during the explosion suppression process, which indicates that potassium ions in SRP are involved in the reaction of ASA and TR gas during the explosion suppression process. Therefore, ASA can efficiently suppress the explosion of TR gas through its chemical inhibition mechanism, primarily by terminating free radical chain reactions.
研究领域:
能源科学
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安全工程
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化学工程
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高影响因子
ChemSusChem
·
2026
·Vol. 19
·期 16
·e70978
·
IF 5.9
Houqiang Shi,Qihui Guo,Liang Lou,Junkai Xiong,Liankang Ye,Lvye Yang,Qiong Peng,Xiang Ge
For treating huge amount of retired lithium‐ion batteries in the coming years, realizing reusability of leachate for the selective recovery of valuable metal elements from spent high‐nickel NCM cathodes is highly desirable, yet it is currently limited by the irreversible degradation of leachate during conventional precipitation processes. Herein, we report the successful realization of reusability for leachate during the selective extraction of transition metal elements using a ChCl:FA DES leachate system. After leaching spent NCM, nickel element can be selectively precipitated by simply cooling. This unique property of reversibly controllable solubility is enabled by the competitive interplay between DES ligands and trace water molecules around the nickel atom. Consequently, Ni elements could be preferentially extracted while Co and Mn could be enriched without adding alkaline precipitating agents, thus enabling leachate reusability. This strategy provides a high recovery yields of 98.73%, 98.09%, and 90.50% for Ni, Co, and Mn respectively. No observable degradation of leachate was observed after three extraction cycles. Our strategy for realizing reusability of leachate for selective recovery of multiple metal elements is expected to offer a general solution with high economic and environmental value for recycling of spent batteries. Precipitant‐free preferential extraction of nickel from spent NCM cathodes is achieved through temperature‐regulated coordination in a ChCl–FA deep eutectic solvent. The reusable leachate enables efficient sequential recovery of Ni, Co, and Mn, providing a simple and sustainable strategy for closed‐loop recycling of lithium‐ion batteries.
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