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CHINESE CHEMICAL LETTERS · 2023 · IF 9.1

Recovery of cathode copper and ternary precursors from CuS slag derived by waste lithium-ion batteries: Process analysis and evaluation

Yun Wei,Lei Zhou,Wenbin Hu,Liming Yang,Guang Yang,Chaoqiang Wang,Hui Shi,Fei Han,Yufa Feng,Xuan Ding,Penghui Shao,Xubiao Luo

The efficient and environmentally friendly recycling technology of waste residue that including abundant heavy metal produced during the recovery of lithium batteries has become a research hotspot. Herein, a novelty process of acid leaching-selective electrodeposition-deep impurity removal-regeneration was proposed to recovery of the CuS slag, which has been efficient transferred to high purity cathode copper and commercially available ternary precursors. Copper cathode with a purity of 99.67% was prepared under electrochemical reaction conditions at −0.55 V for 2 h. A novel impurity remover-Mn powder, which was used to remove the residual impurities and as a feedstock for the ternary precursor. Finally, NCM523 was regenerated by co-precipitation. The process is superior to the traditional process in economy, energy consumption, CO 2 emissions, product purity and process duration. This study provides a new approach for solid waste recovery and precious metal enrichment.

CAS / MDL: 7439-96-5
研究领域: 环境科学 · 材料科学 · 冶金工程
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RENEWABLE & SUSTAINABLE ENERGY REVIEWS · 2022 · IF 16.799

Current challenges and future opportunities toward recycling of spent lithium-ion batteries

Rabeeh Golmohammadzadeh,Fariborz Faraji,Brian Jong,Cristina Pozo-Gonzalo,Parama Chakraborty Banerjee

Lithium-ion batteries (LIBs) are widely used as a critical energy storage system for internet of things (IoT), electric vehicles (EV) and various renewable energy sources . However, the widespread use of LIBs has resulted in the significant accumulation of batteries with different chemistries in landfills. Existing methods for LIB recycling are unsustainable, non-environmentally friendly and ineffective at recycling spent LIBs with mixed chemistry. These methods are inadequate to achieve recovery and repurposing of the valuable and sometimes toxic components. This mandates an inherent need to improve the existing processes or develop a novel, sustainable, environmentally friendly and effective alternative process. In this paper, we present a comprehensive review of the current recovery technologies; demonstrating the gaps in understanding, the challenges and opportunities available in the recycling processes. This review will also examine and discuss different fundamental scientific principles and methods that can be employed to develop sustainable and effective recycling processes with an aim to facilitate the LIB recycling industry to shift towards a circular economy.

CAS / MDL: 12190-79-3
研究领域: 材料科学 · 环境科学 · 能源工程
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Journal of Cleaner Production · 2017 · IF 5.715

An integrated and environmental-friendly technology for recovering valuable materials from waste tantalum capacitors

Bo Niu,Zhenyang Chen,Zhenming Xu

Waste printed circuit boards (WPCBs) are valuable urban ore for recycling. Many efforts have been done to recover resources from basal boards of WPCB. In addition to basal boards, WPCBs contain many electronic components. However, the recycling technology for electronic components has been poorly developed. This study proposed an integrated and environment-friendly technology for recycling waste tantalum capacitors (WTCs) of WPCBs. Firstly, the WTCs were treated by argon pyrolysis to decompose mold resin. The pyrolysis temperature of 550 °C and holding time for 30 min were considered as the optimal parameters. Then, the pyrolysis residues were performed by crush and magnetic separation to recover nickel-iron terminals. Finally, chloride metallurgy (CM) was used to recover rare metal tantalum (Ta). The Ta recovery rate could reach 92.87 ± 0.36%. The optimal parameters were determined as temperature of 493 °C, adding FeCl 2 ·4H 2 O of 53 wt% and holding time for 150 min based on the response surface methodology (RSM). This study exploits an efficient approach for recycling WTCs and provides a reference for future industrial application.

CAS / MDL: 7758-94-3
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Simultaneous peeling of precious metals in cathode and anode of spent ternary batteries using electrolysis

Hui Liu,Xuanrui Huang,Rui Tang,Yulin Min,Qunjie Xu,Zhenhu Hu,Penghui Shi

Recycling spent lithium-ion batteries (LIBs) is of great significance for both environmental protection and resource recycling. However, there are only a few studies on the simultaneous peeling and recycling of battery anode and cathode. Thus, this work proposed a new process for peeling cathode and anode in spent LIBs to solve this problem. The cathode and anode of the spent LIBs were used to form an electrolytic cell to simultaneously realize the peeling of the electrode materials and current collectors and a large amount of Li + leaching. The leaching rate of Li + reached 96.19 % under optimal conditions. In addition, the Li + in the electrolyte can be directly heated and concentrated to be recovered in the form of Li 2 CO 3 . Furthermore, the peeling of cathode materials was caused by the gas shock and defluorination of polyvinylidene fluoride (PVDF). For the Li-free materials, the chemical separation and precipitation method was used to separate and recover Ni, Co, and Mn. In conclusion, this experiment carried out an environmentally friendly electrolysis recycling technique to realize the selective pre-recovery of Li + , the separation of electrode materials with current collectors, and the high purity recovery of current collectors. A new peeling mechanism for the electrolysis recycling technique was also explored. Therefore, this study was expected to provide a useful reference for the electrolysis recycling technique.

CAS / MDL: 5949-29-1
研究领域: 环境科学 · 材料科学
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LANGMUIR · 2023 · IF 3.9

Ecofriendly Viscoelastic Solutions Formed from a Recyclable Rosin-Based Amine Oxide Surfactant

Binglei Song,Hao Chen,Jinpeng Zhang,Zhenggang Cui,Xiaomei Pei

Innovations in molecular structures formed using bioresources are efficient means to prepare surfactant aggregates with unique properties. Here, a rosin-based amine oxide surfactant (R-11-3-AO) containing large hydrophobic groups was synthesized from rosin derivatives, namely, dehydroabietic acid and long-chain amino acids. Cryo-transmission electron microscopy showed that R-11-3-AO molecules formed extremely long wormlike micelles with a cross-sectional diameter of 4–5 nm at a concentration of approximately 7 mmol·L–1. A gel-like system was obtained at approximately 30 mmol·L–1 due to the dense entanglement of the wormlike micelles. The solutions also exhibited unique shear thickening behavior at a shear rate of approximately 10 s–1 even at high concentrations. The large hydrophobic group contained in R-11-3-AO is the origin of the strong van der Waals interactions between the surfactant molecules, resulting in the rapid growth of wormlike micelles. This rosin-based surfactant is the first recoverable amine oxide surfactant from solutions through the salting-out effect with high recovery rates. This work demonstrates the unique capabilities of rosin-based surfactants for forming wormlike micelles and provides opportunities for the development of surfactant recovery technologies.

CAS / MDL: 2432-99-7 109-55-7
研究领域: 材料科学 · 化学工程 · 环境科学
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Journal of Materials Chemistry A · 2024 · IF 10.7

“Polymer to polymer” recycling and body-temperature triggered shape memory of a carvone-based epoxy thermoset system achieved using a thiol-Michael covalent adaptable network

Beitao Liu,Jiahui Li,Cijian Zhang,Yibo Wang,Xigao Jian,Zhihuan Weng

Environmental economics is intensifying the necessity for the advancement of recycling technologies to address the increasing volume of discarded thermoset polymers. Covalent adaptable networks (CANs) provide a new strategy for the recycling and functionalization of thermosetting resins. Herein, a carvone-based CAN is developed, in which thermally driven depolymerization of mechanically robust polymer networks is achieved by dynamic thiol-Michael bonds. The original cross-linking network can be retained through simple drying and hot-pressing steps without purifying degradation products. The reversibility of the thiol-Michael group is demonstrated and the CAN exhibits shape memory behaviors triggered by human body temperature. We propose a micro-robotic injection model with good mechanical strength and fast response speed for complex 1D to 3D shape morphing in aqueous media at 37 °C. Our findings present a high-quality strategy to realize recycling and functionalization of bio-based thermoset resins and expand the toolbox for the preparation of bio-based CANs with thermo-responsive behavior.

研究领域: 材料科学 · 聚合物化学 · 可持续材料 · 回收技术
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ELECTROCHIMICA ACTA · 2025 · IF 5.6

Electrorefining of zinc from hot-dip galvanizing slag in a choline chloride/ethylene glycol based deep eutectic solvent

Haotian Tang,Mengwei Guo,Rongrong Deng,Mingyuan Gao,Qibo Zhang

This study investigates the electrorefining of zinc derived from hot-dip galvanizing (HDG) slag, employing a deep eutectic solvent (DES) composed of choline chloride and ethylene glycol, commonly referred to as Ethaline DES. A thorough electrochemical analysis was carried out to examine the oxidative dissolution behaviors of metallic zinc and associated impurity metals, along with the reduction behavior of Zn(II) ions. These findings demonstrate that, in the Ethaline-ZnCl 2 DES system, zinc undergoes oxidation preferentially compared to impurities, enabling selective extraction of zinc from HDG slag. Furthermore, the reduction potential of Zn(II) is observed to be more positive than that of the impurity metal ions, favoring its preferential deposition at the cathode. Increasing the temperature and incorporating an appropriate quantity of water significantly reduce the viscosity and improve conductivity of the Ethaline DES system, thereby enhancing charge transfer and diffusion of Zn(II) ions while lowering the energy barrier for Zn(II) reduction. Under optimized electrorefining conditions, the resulting cathodic zinc achieves a purity of 99.967 %, with a current efficiency of 95.14 % and an energy consumption of 787 ± 26 kWh/t. This work proposes a sustainable and energy-efficient method for the electrorefining of zinc from HDG slag, presenting a viable pathway for the valorization of this metallurgical byproduct.

研究领域: 冶金学 · 电化学 · 可持续材料加工 · 回收技术 · 绿色溶剂
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JOURNAL OF APPLIED POLYMER SCIENCE · 2025 · IF 2.8

Thermoreversible Behavior of Castor Oil-Based Polyurethane Vitrimer Under Different Dynamic Covalent Networks

Kuiling Wei,Xuejuan Cao,Yan Wu,Xiaoyu Yang,Boming Tang,Tianqiang Jiang

Recycling thermosets is essential for environmental protection and the sustainable development of a circular economy. Among various approaches, dynamic chemistry has proven to be an effective solution for recycling thermosetting polymers. To improve the sustainability of thermosetting polyurethanes and investigate their thermoreversible behavior with different combinations of disulfide bonds and Diels–Alder bonds, this study developed castor oil-based polyurethane vitrimer (Co-PUV 1/Co-PUV 2/Co-PUV 3) with varying dynamic covalent networks. The chemical structure, dynamic reversible reactions, rheological characteristics, and thermal-responsive self-healing were analyzed. The results revealed that disulfide bonds, combined with Diels–Alder bonds, can significantly enhance the thermoreversible response of the crosslinked networks. The first-rank combination was found in Co-PUV 2, which contained Diels–Alder bonds and 4.22 mol% disulfide bonds. This sample exhibited the shortest stress relaxation time and the largest creep range between 60°C and 100°C. Additionally, Co-PUV 2 achieved an 84.4% recovery rate of mechanical properties at 85°C and 0.3 MPa and regained its melt-recyclability at 135°C. In general, this work provides insights into the influence of disulfide and Diels–Alder bonds on the thermoreversible behavior of castor oil-based polyurethane vitrimer, enlightening a foundation for the design of recyclable polyurethane using a multi-dynamic bond strategy.

研究领域: 高分子科学 · 材料化学 · 可持续材料 · 动态共价化学 · 回收技术
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JOURNAL OF HAZARDOUS MATERIALS · 2025 · IF 11.3

Multi-task deep learning meets hyperspectral imaging: A unified modeling framework for WEEE plastic identification and flame retardant quantification

Huihuang Zou,Pinjing He,Fan Lü,Hua Zhang

Rapid plastic identification and additive/contaminant quantitation are critical for efficient recycling of waste electrical and electronic equipment (WEEE). Conventional single-task approaches treat these objectives in isolation, limiting their performance when analyzing high-dimensional spectral data. This study proposes a framework that integrates a multitask convolutional neural network, shared and task-specific learning, and cross-task fusion and attention to simultaneously classify polymer substrates, identify flame retardant types, and quantify flame retardant loading based on hyperspectral imaging data. The dataset comprised laboratory-prepared samples of three common WEEE plastics (acrylonitrile butadiene styrene, high-impact polystyrene, and polypropylene) compounded with four representative flame retardants (ammonium polyphosphate, aluminum trihydrate, decabromodiphenyl ether, and decabromodiphenyl ethane) across graded loadings (1–30 %). The proposed model outperformed single-task baseline models on near-infrared hyperspectral imaging data, improving the classification accuracy of polymer substrates and flame retardant type by 7–10 % and increasing the R 2 score for flame retardant loading regression by 0.04–0.071. Comparable performance gains were achieved using the proposed model on mid-wave infrared data. The findings of the study provide a solid theoretical foundation and technical support for intelligent recognition and efficient sorting of WEEE plastics. Notably, the framework may be adopted in other two-dimensional spectral sensing applications, including solid waste sorting, pollutant monitoring, and broader intelligent environmental sensing.

CAS / MDL: 21645-51-2 84852-53-9
研究领域: 环境工程 · 机器学习 · 光谱成像 · 回收技术 · 材料科学
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Journal of Materials Chemistry A · 2025 · IF 9.5

Direct Regeneration of Cathodes from Spent LIB Black Mass through Integrated Roasting-Flotation with Impurity-Tailored Self-Decontamination

Yuchen Li,Zhengni Ye,Shuai Wang,Hong Zhong,Zhanfang Cao,Xin Ma

Addressing the critical incompatibility between direct recovery technology and industrial battery-crushing technology, this work proposes a short-process, eco-friendly strategy for the direct regeneration of cathode material from spent lithium- ion battery black mass (BM). In the strategy, the cathode material (designated S-NCM) with a 99.08% recovery and a 95.92% grade is firstly extracted greenly and nondestructively via flotation separation after roasting pretreatment. Crucially, residual metal impurities in the BM are ingeniously utilized to capture fluorinated pollutants (e.g., HF) during the roasting process, effectively eliminating hazardous gas emissions. Following targeted prelithiation and high temperature sintering, S-NCM is transformed into regenerated cathode material (R-NCM). Electrochemical tests demonstrate that R-NCM delivers a reversible specific capacity of 139.27 mAh·g−1 at 0.1 C and maintains 91.85% capacity retention after 100 cycles. Techno-economic analysis confirms the strategy’s significant environmental benefits and commercial viability. The total energy consumption of direct regenerating (2.88 MJ·kg−1) is substantially lower than that of pyro-methods (39.12 MJ·kg−1) and hydro-methods (42.97 MJ·kg−1). Owing to its process simplicity, low energy demand, and elimination of secondary synthesis, the regenerated cathode material can directly serve battery remanufacturing. Consequently, the direct regenerating strategy offers 6.8-fold and 2.4-fold higher profitability compared to pyro- and hydro- methods, respectively. This work provides a sustainable solution for large-scale direct regeneration of spent battery-derived BM.

CAS / MDL: 554-13-2 872-50-4
研究领域: 材料科学 · 可持续能源 · 回收技术 · 环境工程 · 电化学
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RARE METALS · 2025 · IF 11

A Dual Closed-Loop Process to Recycle High Nickel Cathode of Spent Lithium-Ion Batteries via Deep Eutectic Solvents: Computational Screening and Experimental Validation

Yang Chen,Shi Luo,Ping Liu,Meng-Fei Chen,Ajanaku Kolawole Oluseyi,Chun-Tao Zhang,Biao Gao,Kai-Fu Huo

en Deep eutectic solvents (DESs) have displayed a significant potential in green recycling of spent lithium-ion batteries (LIBs) cathode materials. In this study, we proposed a computational screening strategy based on the binding energy and hydrogen bonding performance via density functional theory and molecular dynamic calculation, achieving a novel DES system composed of tetramethylammonium chloride (TMAC) and oxalic acid dihydrate (OA) for a dual closed-loop process to recycle LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode of spent LIBs. The binding energy between DESs and Li/Ni/Co/Mn ions were shown to critically influence metal leaching efficiency, implying that DESs with higher binding energy exhibited superior extraction performance. DES TMAC-OA was screened out as optimal potential, and then followed by experimental validations to achieve the leaching of valuable metals from spent NCM811 cathode powder in a much milder condition (80°C, 30 min) with high efficiency. Combined with the coordination regulation of water and ethanol, a high selectivity separation of Li and Ni/Co/Mn can be achieved to regenerate high-value precursors of NCM811 with both high purity and yield. The regenerated precursors can be used to produce new NCM811 with considerable electrochemical performances. More importantly, DESs can be perfectly regenerated and recycled many times, indicating that the process is cost-effective and eco-friendly. Such a strategy provides a feasibility basis to demonstrate a promising potential of DESs in the green recovery and recycling of valuable materials from spent LIBs, therefore benefiting the circular economy and the sustainable management of electronic waste. 摘要 zh 低共熔溶剂(DESs)在退役锂离子电池(LIBs)正极材料的绿色回收方面显示出巨大的潜力。在本研究中,我们提出了一种通过密度泛函理论(DFT)和分子动力学(MD)计算结合能(BE)和氢键性能,用以筛选低共熔溶剂的策略,优选出由四甲基氯化铵(TMAC)和草酸二水合物(OA)组成的DES,可实现退役锂电池NCM811(LiNi 0.8 Co 0.1 Mn 0.1 O 2 )正极材料的双循环回收工艺。DESs和Li/Ni/Co/Mn离子之间的结合能被证明对金属浸出效率有关键影响,而且结合能较高的DESs具有优异的金属浸取性能。浸取实验表明优选出的DES TMAC-OA可以在更温和的条件下(80°C,30分钟)从退役NCM811(S-NCM)正极粉中高效浸出有价金属。结合水和乙醇的配位调节,实现了Li和Ni/Co/Mn的高选择性分离,制备出高纯度和高收率的再生NCM811前驱体。使用再生前驱体可以重新合成出电化学性能优异的新NCM811正极。更重要的是,DES可以多次再生和循环使用,这表明该工艺具有较高的成本效益和环保特性。这一策略为低共熔溶剂从退役锂电池中绿色回收和再生高价值材料方面的巨大潜力提供了可行性基础,从而有利于循环经济和电子废物的可持续管理。

CAS / MDL: 75-57-0
研究领域: 材料科学 · 环境工程 · 可持续能源 · 计算化学 · 回收技术
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JOM · 2023 ·Vol. 75 ·期 9 ·3643-3654 · IF 2.6

Preferential Recovery of Lithium Based on Mineral Phase Reconstruction from Spent Lithium-Ion Batteries

Wang Kai,Zhang Yali,Chen Linlin,Huang Yaoguo

The recovery efficiency of lithium (Li) is low from spent lithium-ion battery in hydrometallurgical recycling because it is recovered in the final procedure. To improve its efficiency, we propose to add thioacetamide in the process of heating separation of cathode active material and Al foil, and the mineral phase of active material has been reconstructed. Li is preferentially recovered by leaching with sodium carbonate solution. The recovery efficiency of Li has been greatly improved. The influence of roasting and leaching conditions was investigated. The results suggest active material has been well separated from Al foil, and the leaching efficiency of Li reaches 97.00% under optimal conditions. The leaching efficiency of Ni, Co and Mn leached by HNO 3 can reach 99.0%. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) reveal the chemical valence of Co and Mn changes and that of Ni remains unchanged in the heating separation.

研究领域: 材料科学 · 回收技术 · 冶金学 · 可持续能源
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