The disposal of hazardous waste of any form has become a great concern for the industrial sector due to increased environmental awareness. The increase in usage of hydroprocessing catalysts by petrochemical industries and lithium-ion batteries (LIBs) in portable electronics and electric vehicles will soon generate a large amount of scrap and create significant environmental problems. Like general electronic wastes, spent catalysts and LIBs are currently discarded in municipal solid waste and disposed of in landfills in the absence of policy and feasible technology to drive alternatives. Such inactive catalyst materials and spent LIBs not only contain not only hazardous heavy metals but also toxic and carcinogenic chemicals. Besides polluting the environment, these systems (spent catalysts and LIBs) contain valuable metals such as Ni, Mo, Co, Li, Mn, Rh, Pt, and Pd. Therefore, the extraction and recovery of these valuable metals has significant importance. In this Review, we have summarized the strategies used to recover valuable (expensive) as well as cheap metals from secondary resources-especially spent catalysts and LIBs. The first section contains the background and sources of LIBs and catalyst scraps with their current recycling status, followed by a brief explanation of metal recovery methods such as pyrometallurgy, hydrometallurgy, and biometallurgy. The recent advances achieved in these methods are critically summarized. Thus, the Review provides a guide for the selection of adequate methods for metal recovery and future opportunities for the repurposing of recovered materials.

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Recycle, Recover and Repurpose Strategy of Spent Li-ion Batteries and Catalysts: Current Status and Future Opportunities

Second life and recycling of retired automotive lithium-ion batteries (LIBs) have drawn growing attention, as large volumes of LIBs will retire in the coming decade. Here, we illustrate how battery...

Second life and recycling: Energy and environmental sustainability perspectives for high-performance lithium-ion batteries.

This review presents a brief scenario about the development of cathodes, anodes, and electrolytes for the next generation of Li-ion batteries (LIBs) and supercapacitors for future energy technologies. Specific capacity...

Progress in Electrode and Electrolyte Materials: Path to All-solid-state Li-ion Batteries (ASSLIB)

用去离子水将原始的LiNi0.8Co0.15Al0.05O2正极材料进行洗涤并分别在不同温度下处理相同的时间, 讨论了LiNi0.8Co0.15Al0.05O2正极材料结构、形貌以及电化学充放电性能的变化, 同时探讨了洗涤和热处理对材料结构、电化学充放电性能以及倍率性能影响的机理。XRD分析表明： 在洗涤和热处理之后, LiNi0.8Co0.15Al0.05O2正极材料的I（003）/I（104）比值以及晶胞体积均有变小; 傅里叶红外光谱分析表明： 在洗涤和热处理之后, LiNi0.8Co0.15Al0.05O2正极材料中形成了碳酸锂、镍化合物杂质及其相关变化。同时对洗涤和热处理前后LiNi0.8Co0.15Al0.05O2正极材料容量和倍率性能进行测试。容量测试结果表明： 原始样品以及处理后样品在30圈循环之后容量保持率分别为88.87%、 87.21%、85.43%和87.80%。

洗涤和热处理对LiNi0.8Co0.15Al0.05O2正极材料结构和电化学充放电性能的影响

One of the main problems of LiNi0.80Co0.15Al0.05O2(NCA) materials is the sidereactions occurring during battery cycling. These side reactions result in capac-ity fading, which in turn decreases the life span of the battery. Conventionally,for nickel-rich cathodes, an inorganic layer is used as a protective layer. Apply-ing these layers may require additional complicated steps. To overcome thisproblem, we focused on coating the NCA electrode with a polymeric ion con-ductive layer that can easily be applied. For this purpose, using an ion-conductive polymer is a novel approach. We used Nafion as the protectivelayer on NCA electrodes. While the Nafion layer can protect the surfaceagainst the side reactions, it does not prevent the Li+ion flow. Following thispurpose, we synthesized NCA by a modified co-precipitation method followedby sintering at 750C. After the preparation of the NCA cathodes, we coatedthe surfaces with a more straightforward drip coating. The Nafion-coated elec-trodes delivered a superior electrochemical performance with 100% of dis-charge capacity retention even after 100 cycles at 0.1C. The electrochemicalimpedance spectroscopy revealed that the Nafion coating could effectively pre-vent passive layer formation, which causes capacity fading.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/est2.154

Nafion-coated LiNi0.80Co0.15Al0.05O2 (NCA) cathode preparation and its influence on the Li-ion battery cycle performance

An approach for a fast recycling process for Lithium Nickel Cobalt Aluminum Oxide (NCA) cathode scrap material without the presence of a reducing agent was proposed. The combination of metal leaching using strong acids (HCl, H2SO4, HNO3) and mixed metal hydroxide co-precipitation followed by heat treatment was investigated to resynthesize NCA. The most efficient leaching with a high solid loading rate (100 g/L) was obtained using HCl, resulting in Ni, Co, and Al leaching efficiencies of 99.8%, 95.6%, and 99.5%, respectively. The recycled NCA (RNCA) was successfully synthesized and in good agreement with JCPDS Card #87-1562. The highly crystalline RNCA presents the highest specific discharge capacity of a full cell (RNCA vs. Graphite) of 124.2 mAh/g with capacity retention of 96% after 40 cycles. This result is comparable with commercial NCA. Overall, this approach is faster than that in the previous study, resulting in more efficient and facile treatment of the recycling process for NCA waste and providing 35 times faster processing.

A Fast Metals Recovery Method for the Synthesis of Lithium Nickel Cobalt Aluminum Oxide Material from Cathode Waste

Zinc oxide (ZnO) is one of the most promising materials applied in Li-ion batteries. In this research, ZnO was synthesized by the thermal decomposition of zinc oxalate dihydrate. This precursor was obtained from the precipitation process of zinc sulfate with oxalic acid. In-depth studies were carried out on the effect of various heating temperatures of zinc oxalate dihydrate precursors on ZnO synthesis. The as-prepared materials were characterized by XRD, SEM, and FTIR. Based on the XRD analysis, the presence of the ZnO-wurtzite phase can be confirmed in samples heated at temperatures above 400 °C. Meanwhile, SEM-EDX results showed that the ZnO particles have a micron size. Cells with ZnO samples as anodes have low columbic efficiency. In contrast, cells with ZnO/Graphite composite anodes have a relatively large capacity compared to pure graphite anodes. Overall, based on the consideration of the characterization results and electrochemical performance, the optimal sintering temperature to obtain ZnO is 600 °C with a cell discharge capacity of ZnO anode and in the form of graphite composites is 356 mAh/g and 450 mAh/g, respectively. This suggests that ZnO can be used as an anode material and an additive component to improve commercial graphite anodes’ electrochemical performance.

Synthesis and Characterization of ZnO from Thermal Decomposition of Precipitated Zinc Oxalate Dihydrate as an Anode Material of Li-Ion Batteries

Spent nickel catalyst will be harmful to the environment if it is not processed or used properly. In fact, this waste still has a high nickel content. The treatment of spent nickel catalysts has been widely reported, but limited to nickel extraction. Since the lithium-ion batteries demand is continued to increase, then nickel is the most sought-after metal. Consequently, nickel from spent nickel catalysts could be developed as secondary source for lithium-ion battery cathode. This study aims to utilize spent nickel catalysts into more valuable materials. Nickel that has been extracted and mixed with Mn and Co has been used as raw material for nickel-rich cathode, namely NMC. Nickel extraction and NMC synthesis were using the acid leaching method followed by co-precipitation [WI1] [SSN2]  . Based on the functional test performed in this work, nickel from spent nickel catalyst can be applied to Li-ion batteries. The sintering temperature that gives good characteristics and electrochemistry was found 820 o C. The galvanostatic charge-discharge test gave specific capacity results for NMC of 110.4 mAh/g. The cycle test showed that NMC synthesized from spent nickel catalyst can be carried out up to 50 cycles with a capacity retention of 87.18%.

Utilization of Spent Nickel Catalyst as Raw Material for Ni-Rich Cathode Material

Fe based catalysts for petroleum coke graphitization for Lithium Ion battery application

Significant demand of Li-ion batteries (LIBs) is raising awareness of future LIBs wastes which are highly required to be reprocessed, reused or recycled. In this research, copper foil waste from spent LIBs are upcycled as an anode material, CuO. Hydrometallurgical route was applied to selectively dissolve copper foils where nitric acid, maleic acid and acetic acid were used as the leaching agents while oxalic acid were used to precipitate copper into copper oxalate which is a precursor to CuO. CuO was obtained by calcination of copper oxalate at high temperature. Based on XRD and FTIR analysis, Copper (II) oxalate dihydrates is successfully obtained while SEM images of the samples confirmed micron sized agglomerates which is consist of submicron primary particles. XRD analysis of CuO samples obtained from various leaching process confirmed that a pure CuO is successfully synthesized from nitric acid leaching process while CuO from acetic acid and maleic acid leaching has Cu2O and Cu phase. CuO and 10%CuO@graphite sample from nitric acid leaching were used as sole anode and composite anode in a LiNi0.8Co0.1Mn0.1O2(NCM) battery, respectively. The initial columbic efficiency of CuO anode was far inferior to CuO@graphite. However, CuO@graphite had higher specific charge-discharge capacity with the value of 347.8 mAh/g compared to pure graphite (286.5 mAh/g). In conclusion, Cu-foils are a promising source of CuO to enhance the capacity of commercial graphite anode.

Hanida Nilasary

Papers

A Fast Metals Recovery Method for the Synthesis of Lithium Nickel Cobalt Aluminum Oxide Material from Cathode Waste

Synthesis and Characterization of ZnO from Thermal Decomposition of Precipitated Zinc Oxalate Dihydrate as an Anode Material of Li-Ion Batteries

Utilization of Spent Nickel Catalyst as Raw Material for Ni-Rich Cathode Material

Fe based catalysts for petroleum coke graphitization for Lithium Ion battery application

Utilization of Cu-Foil Waste as a High-Capacity Anode Material for High Performance LiNi0.8Co0.1Mn0.1O2/ CuO@Graphite Batteries