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JOM · 2022 ·Vol. 74 ·期 5 ·1934-1944 · IF 2.597

Efficient Oxidation Approach for Selective Recovery of Lithium from Cathode Materials of Spent LiFePO4 Batteries

Liu Peiwen,Fei Zitong,Zhang Yingjie,Dong Peng,Meng Qi,Yang Xi

Developing a green and efficient approach for recovering Li from cathode materials is important in recycling spent LiFePO 4 batteries. A facile and efficient oxidation process was developed to selectively recover Li from spent LiFePO 4 batteries. The common oxidant NaClO was used to avoid using acid or alkali in the leaching process. The leaching rate of Li reached 99.8% under the selective optimal leaching conditions of 0.54 mol/l NaClO, leaching time 60 min, leaching temperature 60°C and solid–liquid ratio 1 g/l. The high leaching efficiency can be ascribed to the combination of oxidability and high pH value of the NaClO solution. Meanwhile, leaching and precipitation were carried out simultaneously in this process, which promoted the leaching reaction. High performance LiFePO 4 /C was resynthesized using the recovered products. The specific capacity of the first discharge at 1 C was 147.1 mAh/g and the capacity retention rate at 1 C was 97.55% after 200 cycles. The oxidation approach is acid free and has low energy consumption for green recovery of spent LiFePO 4 batteries.

研究领域: 材料科学 · 环境科学 · 能源技术
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GREEN CHEMISTRY · 2024 · IF 9.3

Green palladium and platinum recovery by microwave-assisted aluminum chloride solution

Anting Ding,Chuanying Liu,Chengliang Xiao

Palladium and platinum are precious metals (PMs) used in industrial catalysis, and their green recycling is crucial but challenging. In this study, we aimed to create a novel leaching procedure for the environmentally friendly recovery of PMs using AlCl3·6H2O solution. We report here the use of a microwave-assisted AlCl3·6H2O solution to selectively recover Pd and Pt from spent catalysts. In a large-scale setting, our system can recover gram-scale Pd in a single batch. Electron paramagnetic resonance (EPR) and capture experiments revealed the hydroxyl radicals produced by proton dissociation and microwave coordination triggered the oxidative dissolution process. Microwave-assisted AlCl3·6H2O solution leaching and NaBH4 reduction recovered high-purity Pd and Pt separately. In scale-up experiments, the dissolution performance of the microwave-assisted AlCl3·6H2O solution for Pd remained almost unchanged after seven cycles. Our approach uses around 1/50 and 1/20 of the energy and chemical inputs of the conventional hydrometallurgy process, respectively. Strong acids, poisonous cyanide, and volatile organic solvents were not used during the recovery process, enabling an efficient and sustainable PM recovery process and promoting an advanced oxidation process (AOPs) technology for secondary resource recycling.

研究领域: 化学工程 · 环境科学
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ACS ES&T Engineering · 2022 · IF 0

Aqueous Photocatalytic Recycling of Gold and Palladium from Waste Electronics and Catalysts

Jiazhen Cao,Yao Chen,Hengjun Shang,Xiang Chen,Qianyu Qiao,Hexing Li,Zhenfeng Bian

Gold and palladium are the most widely used precious metal materials in the field of electronic devices and industrial catalysis. How to realize the green recycling of gold and palladium is important and challenging. In this work, we found that gold and palladium in wastes, such as electronic devices and industrial catalysts, can be completely dissolved and recycled by photocatalysis. Gold and palladium are oxidized to the ionic state in water, which does not involve strong acids, strong alkalis, toxic cyanides, or an organic medium. More interestingly, the dissolution of gold and palladium in different halogen aqueous solutions has special selectivity, which depends on the coordination stability constants between gold and palladium with halide ions. Therefore, gold and palladium can be selectively dissolved in iodine ion solution and bromine ion solution, respectively, then gold and palladium can be obtained by a one-step reduction. This work opens up a new direction for optimizing the photocatalytic dissolution technology and promoting the green recycling of precious metals.

研究领域: 环境科学 · 材料科学
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POLYMER DEGRADATION AND STABILITY · 2024 · IF 6.3

Catalytic upcycling of silicone rubber by AlCl3 at low temperature

Kemeng Liu,Xueying Wen,Huiyue Wang,Huajian Liu,Lijie Liu,Ran Niu,Tao Tang,Nan Yao,Ruikun Pan,Jiang Gong

Chemical recycling of silicone rubber (SR) waste into valuable products has aroused ever-increasing attention; however, the development of a green, efficient degradation strategy for silicone rubber remains challenging. In this work, we report the catalytic upcycling of silicone rubber by AlCl 3 to produce SiO 2 under atmospheric environment. The optimized AlCl 3 /SR mass ratio, reaction temperature and time are 0.75, 280 ℃ and 120 min, respectively. The maximum yield of SiO 2 is 96 %. The as-prepared SiO 2 displays irregular spherical agglomerates with a particle size of 20–30 nm and bears rich micropores/mesopores/macropores. The result of variable-temperature Fourier-transform infrared spectroscopy proves that AlCl 3 promotes the fracture of Si-O in SR during heating. According to density functional theory, the addition of AlCl 3 leads to a decrease in the bond dissociation energy of Si-O and Si-C. The strategy achieves the green, efficient catalytic degradation of silicone rubber waste.

研究领域: 材料科学 · 化学工程
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Journal of Cleaner Production · 2022 · IF 11.072

Novel layered iron antimony thiostannate adsorbent of K1.61Fe0.04Sb0.03Sn3.1S7 for cesium green recovery from geothermal water

Zhenzhen Jiang,Chi Ma,Yanqing He,Mingli Li,Gaoling Liu,Yafei Guo,Duo Ji,Tianlong Deng

To develop a green and efficient cesium adsorbent with high adsorption capacity , rapid kinetics, and good regeneration performance is a tremendous challenge. In this work, potassium iron antimony thiostannate (PIATS) synthesized by the hydrothermal method was utilized for green recovery cesium from geothermal water for the first time. PIATS showed a high adsorption capacity of 401.23 mg/g, which was much higher than other types of adsorbents at present. Meanwhile, PIATS showed rapid ion exchange kinetics (within 3 min) and broad pH resistance (4–12). More importantly, PIATS still showed excellent selectivity to cesium even in geothermal water containing many other coexisted ions ( K d  = 1.96 × 10 4  mL/g), and the separation factors between Cs + and the coexisted competing ions were ranged from 462.77 to 963.76. Subsequently, the cesium-laden PIATS could be easily eluted with 0.50 mol/L NaNO 3 to achieve rapid desorption (within 10 min). The concentration of Cs + in the elution was enriched more than 11 times higher than that in the original solution. Furthermore, no organic solvents or other toxic reagents were involved during the whole process. Therefore, the adsorption advantages, excellent enrichment ability, and structural stability of PIATS make it a potential recyclable candidate for green cesium recovery from geothermal water.

研究领域: 环境科学 · 材料科学
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JOURNAL OF POLYMERS AND THE ENVIRONMENT · 2025 · IF 5

Hydrolysis in PET Alcohol Salt Systems: Exploration of Novel Catalytic Pathways

Cui Panpan,Ge Chao,Shi Sheng,Zhang Meiling,Su Qianyu,Hou Wensheng

The production and disposal of polyester fibers have been rapidly increasing, highlighting the urgent need for green and efficient recycling technologies to promote fiber resource circularity. Although the conventional alkaline hydrolysis method for polyester offers a simple process, its reliance on strong alkaline media and high-temperature conditions leads to severe equipment corrosion, high energy consumption, and significant secondary pollution risks, greatly limiting its large-scale application. In this study, an innovative ethanol-sodium carbonate (EtOH-Na₂CO₃) synergistic catalytic system was developed. By leveraging the cooperative effects of an organic–inorganic hybrid solvent, PET was efficiently depolymerized under mild conditions. The results indicate that when the alcohol-to-water ratio was optimized to 1:1 (v/v), the catalyst loading (Na₂CO₃/PET) was set at 2:3 (w/w). The reaction was conducted at 150 °C for 105 min; PET was completely converted, achieving a terephthalic acid (TPA) yield of up to 98%, five times higher than that of traditional non-alcoholic systems. Moreover, this method was also applicable to colored polyester fibers, producing TPA that met industrial-grade standards. These findings demonstrate the great potential of this approach for large-scale applications. This study not only elucidates the synergistic catalytic mechanism of the organic–inorganic hybrid solvent system but also establishes a technological bridge from fundamental research to industrial application. It provides an innovative strategy for the closed-loop management of chemical fibers. It offers a novel solution for the high-value recovery of complex fiber waste, thereby facilitating the deep integration of green chemical processes and circular economy models. Graphical

CAS / MDL: 104-76-7
研究领域: 化学工程 · 环境科学 · 材料科学
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ACS Sustainable Chemistry & Engineering · 2018 · IF 6.14

Reclamation and Harmless Treatment of Waste Cathode Ray Tube Phosphors: Novel and Sustainable Design

Xiaofei Yin,Jiamei Yu,Yufeng Wu,Xiangmiao Tian,Wei Wang,Yi-Nan Zhang,Tieyong Zuo

In this paper, we propose a novel and sustainable process for recycling rare earths (REs) and zinc (Zn) simultaneously from waste cathode ray tube (CRT) phosphors. First, 95% of the impurities such as glass cullets and aluminum foils are removed by simple screening. Then, a self-propagating, high-temperature synthesis reaction following a water-leaching process is performed to recycle Zn selectively. The REs are recycled by a combined process of oxidative leaching and ionic-liquid-based extraction. They are then regenerated to form a new Y2O3:Eu3+ phosphor. By following this green recycling design, the recovery efficiencies of REs and Zn reach 99.5% and 99%, respectively. The negative bivalent sulfur in ZnS and Y2O3:Eu3+ is converted completely to SO42–, which efficiently avoids the secondary pollution. It should also be pointed out that the main recovery processes are all carried out at room temperature, and the “three wastes” emissions are minimized throughout the process. This work is expected to open new avenues for highly efficient, energy-saving, and pollution-reducing recovery processes for waste CRT phosphors.

CAS / MDL: 1314-98-3
研究领域: 材料科学 · 环境科学
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Mechanistic investigation of intensified separation of molybdenum(VI) and vanadium(V) using polymer inclusion membrane electrodialysis

Yuzhen Wang,Pengfei Wang,Huihui Xie,Ming Tan,Lingyun Wang,Yang Liu,Yang Zhang

The main challenge in separating molybdenum(VI) and vanadium(V) which have similar properties results in great difficulties in the green recycling of hazardous spent catalysts. Here, selective facilitating transport and stripping are integrated into the polymer inclusion membrane electrodialysis process (PIMED) to separate Mo(VI) and V(V) to overcome the complicated co-extraction and stepwise-stripping in conventional solvent extraction . The influences of various parameters, the selective transport mechanism, and respective activation parameters were systematically investigated. Results revealed that the affinity of the Aliquat 36 as the carrier and PVDF-HFP as the base polymer of PIM towards Mo(VI) is stronger than that of V(V), while the strong interaction between Mo(VI) and carrier caused low migration through the membrane. By the combination of adjusting and controlling the electric density and strip acidity, the interaction was destroyed and the transport was facilitated. After optimization, stripping efficiencies of Mo(VI) and V (V) increased from 44.4% to 93.1% and reduced from 31.9% to 1.8%, respectively, while their separation coefficient increased 16.3 times to 333.4. The activation energy, enthalpy and entropy for the transport of Mo(VI) were determined to be 4.846 kJ mol −1 , 6.745 kJ mol −1 and − 310.838 J mol −1 K −1 , respectively. The present work demonstrates that the separation of similar metal ions could be improved by fine tuning the affinity and interaction between metal ions and the PIM, thus providing new insights into the recycling of similar metal ions from secondary resources.

CAS / MDL: 63393-96-4 5137-55-3
研究领域: 环境科学 · 材料科学 · 化学工程
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2025 · IF 2.9

Green recovery of solid electrolytes from all-solid-state lithium-ion batteries by low-melting mixture solvents with tunable physical properties

Yu Chen,Xueqing Zhang,Chenyang Wang,Zhuojia Shi,Xihou Wang,Jiayi Dong,Yanlong Wang,Minghui Feng

All-solid-state lithium-ion batteries (ASSLIBs) are anticipated to be the next generation of high-performance lithium batteries due to their enhanced safety and high energy density. However, the widespread application of ASSLIBs will lead to a significant increase in spent batteries, resulting in environmental pollution and resource depletion. Therefore, the development of environmentally friendly recycling methods for ASSLIBs is both urgent and critical. Low-melting mixture solvents (LoMMSs) are proposed by Professor Yu's research group at Tsinghua University in 2023 to facilitate the advancement of green solvents and green chemistry. Here, we utilized LoMMSs to leach metals from solid-state electrolytes (SSEs) of ASSILBs and apply the 55 anti-solvents method to recover metal ions from leachate. Results show that the leaching efficiency of Li is up to 92.5 % at the mild temperature of 80 oC within 24 h. The high Li leaching efficiency is ascribed to the coordination interaction. Furthermore, the Li leaching efficiency in large-scale applications shows minimal deviation from the optimal efficiency. This research provides valuable insights into the development of efficient, green, and mild recycling methods for SSEs in ASSLIBs.

研究领域: 材料科学 · 环境科学 · 化学工程
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MINERALS ENGINEERING · 2021 · IF 4.765

Comprehensive utilization of waste residue from lithium extraction process of spodumene

Xu Wang,Haisheng Hu,Meitang Liu,Yunfei Li,Yong Tang,Lun Zhuang,Benjun Tian

In this work, the comprehensive utilization of spodumene waste residue - lithium slag is achieved. An experimental scheme of hydrothermal preparation of nano-kaolinite and xonotlite from it is proposed. The W-lithium slag is completely decomposed into sodalite and then transformed into hydroxycancrinite in 6 mol/kg NaOH solution at 220 ℃. As an intermediate product, hydroxycancrinite was reacted with 0.65 mol/kg HNO 3 solution at 260 ℃ for 24 h to prepare nano-kaolinite successfully. The desiliconization filtrate produced by the reaction of W-lithium slag and NaOH solution was used as raw material, mixed with CaO and reacted at 260 ℃ for 12 h after aging for 12 h, then xonotlite was successfully prepared. This work demonstrates great potential on green recycling of spodumene waste residue from lithium extraction process and introduce a new economical processing technique for the slag as well.

CAS / MDL: 7697-37-2 1310-73-2
研究领域: 材料科学 · 环境科学
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Industrial Chemistry & Materials · 2025 · IF 11.9

Green recovery of all-solid-state sodium-ion batteries/lithium-ion batteries by ionic liquids, deep eutectic solvents and low-melting mixture solvents

Yu Chen,Guojian Zhao,Jiayi Dong,Jing Wang,Dexin Dong,Zheng Li,Mengxi Zhao,Zhuojia Shi,Zihang Niu

All-solid-state sodium-ion batteries (ASIBs) has good application prospects due to the high energy density, high safety and long lifetime. The excessive use of ASIBs in the near future will inevitably lead to environmental pollution, resources waste and cost increase. In this work, we utilize three types of green solvents—ionic liquids (ILs), deep eutectic solvents (DESs), and low-melting mixture solvents (LoMMSs)—to recover both the cathode materials and solid electrolyte from ASIBs, as well as the cathode and electrolyte from lithium-ion batteries (LIBs). Result shows that the leaching efficiency of Na from the cathode material and solid electrolyte of ASIBs by LoMMSs could respectively reach as high as 92.8% and 96.7% at the mild temperature of 80 oC, which is higher than that in ILs and DESs. The highest metal leaching efficiency from ASIBs is similar to that from LIBs. Both the LoMMSs and leachate investigated are non-flammable when exposed to high-temperature torch. In addition, 70 anti-solvents are screened to recover metal from the leachate at room temperature, with acetone yielding the highest precipitation efficiency of 92%.

CAS / MDL: 107-21-1 57-13-6
研究领域: 材料科学 · 能源工程 · 环境科学
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ChemSusChem · 2024 · IF 7.5

Natural Low-Melting Mixture Solvents for Green Recovery of Spent All-Solid-State Sodium-Ion Batteries with Superior Efficiency over Lithium-Ion Batteries

Yu Chen,Yaxue Shen,Zicheng Liu,Mingshuai Yang,Yuqing Zhang,Zihang Niu,Yanlong Wang,Minghui Feng,Zhuojia Shi

Graphical Natural low-melting mixture solvents could be used to achieve mild, safe and efficient recovery of all-solid-state electrolyte and cathode from all-solid-state sodium-ion batteries with high selectivity. Moreover, water is found to be the green and low-cost anti-solvent to precipitate the extracted metal from the leachate with low-energy consumption at room temperature. Spent all-solid-state sodium-ion batteries (ASIBs) containing toxic and precious metal would be produced significantly and lead to resource waste and environmental pollution as the wide application of ASIBs in the near future. Therefore, it is necessary to develop green strategy for recovery of ASIBs. Here, we propose a safe, mild and green strategy to recover toxic and precious metals from cathode/solid electrolyte of ASIBs by using natural low-melting mixture solvents (LoMMSs) with high selectivity and high leaching efficiency. Natural LoMMSs are abundant, natural available, cheap, non-flammable, biodegradable and biocompatible. Results show that natural LoMMSs could leach nearly 100 % Na and achieve superhigh Na/Zr selectivity of up to 58 from ASIBs at mild temperature, outperforming the recycling efficiency and selectivity of lithium-ion batteries cathode. More importantly, we find that water could be used as a green and low-cost anti-solvent to precipitate the extracted metal from the leachate with low-energy consumption at room temperature. This work provides a cost-effective, energy-saving, mild, green strategy for the recovery of cathode/solid electrolyte from spent ASIBs with high safety and high selectivity.

研究领域: 材料科学 · 环境科学
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