Journal of Energy Chemistry
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2021
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IF 9.676
Tingting Liu,Sheng Cai,Genfu Zhao,Zhihui Gao,Shuming Liu,Huani Li,Lijuan Chen,Mian Li,Xiaofei Yang,Hong Guo
Along with the continuous consumption in lithium-ion batteries (LIBs), the price of cobalt is inevitably going up in recent years. Therefore, recycling valuable Co element from spent devices, and boosting its service efficiency are becoming two indispensable approaches to promote the utilization of Co in various energy conversion/storage devices. Herein, we realize the recovery of Co from spent LIBs and synthesize a three–dimensional (3D) sea-urchin-like cobalt nitride composite material (labeled as CoN-Gr-2), which is used as a bi-functional catalyst for water splitting. Benefiting from the intrinsic high conductivity, larger surface area and unique 3D sea–urchin–like architecture, CoN-Gr-2 shows an excellent electron transfer efficiency, highly exposed active sites as well as the superior mass transport capacity. The CoN-Gr-2 catalyst exhibits low overpotentials of 128.9 mV and 280 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which are comparable to the commercial 20 wt% Pt/C and RuO 2 catalysts. Moreover, when adopting CoN-Gr-2 as both anode and cathode materials for overall water splitting (in 1.0 M KOH electrolyte), the assembled cell achieves a current density of 10 mA cm −2 at 1.61 V, which almost close to that of Pt/C||RuO 2 benchmark (1.60 V), demonstrating its superior water-splitting efficiency. Meanwhile, the CoN catalysts exhibit strong chemical interaction with the Gr support, suppressing the aggregation of CoN catalysts and maintains their high activity during HER and OER reactions. So, the cell exhibits a high current retention of 97.3% after 40 h. This work successfully develops an industrial chain from recycling Co wastes in spent energy devices to controllably designing 3D sea-urchin-like CoN-Gr with high water splitting efficiency. Therefore, it could further promote the efficient utilization of valuable Co element in various energy devices.
研究领域:
材料科学
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能源工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
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IF 7.4
Yongbo Yu,Xiaohua Li,Shanshan Shao,Pengfei Zhang,Jiaxin Jiang
Biomass pyrolysis and in-line steam reforming for hydrogen production is one of the effective ways to promote the sustainable development of global energy. In this study, Co was recovered from the cathode material of LiCoO 2 batteries using the carbon thermal reduction method, and used for biomass pyrolysis and in-line steam reforming for hydrogen production. First, the cathode material was reduced using coconut shell carbon (CC), and it was revealed that cobalt presented in the catalyst prepared at the reduction temperature of 800 °C, giving the hydrogen yield of 24.9 mmol/g. Other carbon source like graphite carbon (GIC) and straw pyrolytic carbon (SC) were then investigated and it was found that a much higher temperature (>800 °C) was required for the reduction of the cathode material with GIC and the catalyst prepared by SC reduction was less effective than that using CC reduction. Considering the great influence of the pore structure of the carbon material on the reduction, activated carbon (AC) was obtained from SC using KOH activation. With a better distribution of cobalt on the carrier prepared by AC reduction, the highest hydrogen yield of 28.3 mmol/g was achieved with the mass ratio of cathode material and AC of 10:3. This study provides a viable avenue for the application of spent lithium-ion battery cathode materials in the production of hydrogen from biomass.
研究领域:
能源科学
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催化化学
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环境工程
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Zhuang Wang,Mian Li,Bin Fu,Wenping Cao,Xiangjie Bo
Although cobalt nitride (CoN)-based nanomaterials have been widely designed as advanced oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and oxygen reduction reaction (ORR) catalysts, the continuous consumption of lithium-ion batteries (LIBs) has led to a high price of cobalt metal. Therefore, in the future, recycling valuable Co elements from spent devices and boosting their service efficiency will inevitably promote the utilization of Co-based materials in water splitting and zinc-air batteries (ZABs). Herein, we realize the Co recycling from spent LIBs by a simple hydrometallurgy method. Under the assistance of hexamethylenetetramine and polystyrene spheres, after the hydrothermal and pyrolysis treatment in the NH 3 atmosphere, the as-reclaimed cobalt oxalates were successfully transformed into novel three-dimensional (3D) CoN nanoflowers (denoted as CoN NFs). Benefiting from the unique 3D flower-like architectures, intrinsic high conductivity, large surface area, uniformly dispersed CoN nanoparticles, and the synergistic effect between Co 3 N and CoO phases, the 3D flower-like CoN NFs exhibited excellent OER catalytic activity. The performance was much better than commercial RuO 2 in the 1.0 M KOH solution. Furthermore, the CoN NFs-based water splitting cell needed a voltage of 1.608 V to achieve the current density of 10 mA cm −2 , which is even 16 mV smaller than that of Pt/C||RuO 2 benchmark (1.624 V). Meanwhile, the CoN NFs-derived ZAB exhibited a high peak power density of 107.3 mW cm −2 (vs. 103.2 mW cm −2 of Pt/C-RuO 2 -based ZAB) and a low charge–discharge voltage gap (0.93 V vs. 1.43 V of Pt/C-RuO 2 -based ZAB). Due to the excellent structural and elemental stabilities, the corresponding water splitting cell and ZAB had outstanding durability. This work successfully explored an advanced industrial chain from recycling Co metal in spent devices to designing the high-efficiency HER/OER/ORR electrocatalysts for advanced water splitting devices and ZABs. This will further promote the value-added utilization of valuable Co metal in various energy storage or conversion devices.
研究领域:
材料科学
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能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Jiefeng Xiao,Bo Niu,Zhenming Xu
The rapid development of new energy technology leads to explosive growth of lithium-ion batteries (LIBs) industry which greatly alleviates the problems of environmental pollution and energy shortage. However, how to realize resource circulation of critical metals including lithium (Li) and cobalt (Co) becomes the new problem of LIBs industry. This paper proposes an improved thermal reduction technology to efficiently recycle Li and Co from spent LIBs, where cheap urea is applied as the only additive to provide ammonia (NH 3 ). By thermal reduction, LiCoO 2 was thermally reduced into water-soluble lithium carbonate and water-insoluble cobalt metal Under the optimal conditions, 99.96% Li with nearly 100% selectivity was obtained by water leaching. More importantly, the concept of “oxygen elements removal (OER)” was proposed to explain the metal extraction from spent LIBs, which could help to describe the reaction mechanism as O-cage digestion mechanism. Furthermore, metal extraction from spent LIBs was re-understood as “seeking an applicable reductant”, which provided a fresh perspective for understanding Li selective recovery. These concepts and findings can provide some inspiration for metal recovery from spent LIBs.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Xiaojian Liao,Maoyou Ye,Jialin Liang,Zhijie Guan,Shoupeng Li,Yanghong Deng,Qiaowei Gan,Zihang Liu,Xiaodi Fang,Shuiyu Sun
The recovery of metals from spent LiCoO 2 batteries (SLBs) is essential to avoid resource wastage and the production of hazardous waste . However, the major challenge in regard to recovering metals from SLBs using traditional bioleaching is the low Co yield. To overcome this issue, a mixed culture of Acidithiobacillus caldus and Sulfobacillus thermosulfidooxidans was designed for use in SLBs leaching in this study. With the assistance of Fe 2+ as a reductant, 99% of Co and 100% of Li were leached using the above mixed-culture bioleaching (MCB) process, thus solving the problem of low metal leaching efficiency from SLBs. Analysis of the underlying mechanism revealed that the effective extraction of metals from SLBs by the Fe 2+ -MCB process relied on Fe 2+ -releasing electrons to reduce refractory Co(III) to Co(II) that can be easily bioleached. Finally, the hazardous SLBs was transformed into a non-toxic material after treatment utilizing the Fe 2+ -MCB process. However, effective SLBs leaching was not achieved by the addition of Fe 0 to the MCB system. Only 25% Co and 31% Li yields were obtained, as the addition of Fe 0 caused acid consumption and bacterial apoptosis. Overall, this study revealed that reductants that cause acid consumption and harm bacteria should be ruled out for use in reductant-assisted bioleaching processes for extracting metals from SLBs.
研究领域:
环境科学
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微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jiateng Shi,Junfeng Wang,Tao Dong,Jie Yan,Danfeng Jiang,Zengxi Li,Haitao Zhang
The ionic liquid tetrakis(decyl)ammonium dicyanamide ([TKN][Dca]) was investigated for the selective extraction of Co(II) from a simulated spent battery leachate, achieving efficient separation of Co(II) from Ni(II) and Li(I). [TKN][Dca] demonstrate a high Co(II) extraction efficiency in a 4 mol/L NaCl solution, without requiring pH adjustment. The separation factor ( β Co/Ni ) for [TKN][Dca] was determined to be 47433. Density functional theory (DFT) calculations and ESI-MS spectra revealed that the predominant anionic species involved in Co(II) extraction were [Co(Dca) 3-x Cl x ] − , with [Co(Dca)Cl 2 ] − and [Co(Dca) 2 Cl] − as the primary complexes. The strong coordination between the dicyanamide anion (Dca − ) and Co(II) enabled selective separation of Co(II) from the leachate. Co(II) was efficiently stripped from the loaded organic phase using Na 2 SO 4 , with the extraction efficiency after stripping comparable to that of fresh [TKN][Dca]. Furthermore, [TKN][Dca] exhibits excellent stability and maintained consistent performance over multiple extraction-stripping cycles, highlighting its potential for sustainable applications in metal separation fields.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Chuhan Tang,Wei Shan,YiRan Zheng,Liang Zhang,Yuxin Liu,Bin Liao,HeDong Chen,Xianhua Hou
The widespread application of Lithium-ion Batteries (LIBs) has led to a significant increase in the number of spent LIBs. Consequently, the recycling and utilization of spent LIBs have become an inevitable choice for recovering valuable resources and protecting the environment, aligning with the principles of sustainable development. This study reports an iron air battery recycling system that is capable of recovering both Li/Co and energy from spent LiCoO 2 cathode materials and the separation reaction is completely spontaneous. Meanwhile, lithium and cobalt were successfully recovered from the powdered leach solution of spent LiCoO 2 cathode material, and it was preliminarily demonstrated that spent iron could be used as a sacrificial anode for the system. Several key parameters affecting recovery are optimized, including anode solution pH, discharge current density, and concentration of the solution to be recovered. Under the conditions of anode solution pH of 1.8, discharge current density of 0.1 mA cm −2 , and concentration of recovery solution of 0.15 mol/L, the system can be operated stably for more than 24 h, and the recoveries of Li + and Co 2+ can be up to 1.49 mg h −1 and 18.75 mg h −1 respectively, and the output energy can reach 75.15 kJ/mol. This research not only provides a sustainable and cost-effective method of disposing of used lithium-ion batteries, but also offers up new possibilities for the disposal of scrap iron.
研究领域:
环境科学
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材料科学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
JOM
·
2025
·
IF 2.3
Yin Ning,Song Yonghui,Zhang Xingyu,Dong Ping,Zhang Xinwei
We aimed to recover Ni and Co from the leaching sulfate solution of nickel-based superalloy scraps (NSL) and to synthesize NiCo 2 O 4 through oxalate co-precipitation-calcination technique. The structural and compositional analyses of the resultant products were characterized utilizing x-ray diffraction (XRD), x-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM). Furthermore, the effects of nickel-cobalt molar ratio and calcination temperature on the oxygen evolution reaction (OER) performance were investigated. The results indicated that under optimal conditions of 0.7 M C 2 O 4 2− addition, 25°C, and 4 h reaction time, the precipitation efficiencies for Co 2+ and Ni 2+ were 99.19% and 95.79%, respectively. The precipitate derived from adjusting the Ni/Co molar ratio in NSL manifested as a solid solution of nickel-cobalt oxalate (Ni x Co 3-x (C 2 O 4 ) 3 ). As the molar ratio decreased, the precipitates gradually transformed from a nickel oxalate structure with Ni sites replaced by Co to a cobalt oxalate structure with Ni replacing Co sites. The pure phase structure NiCo 2 O 4 , synthesized with a Ni/Co molar ratio of 1/2 and calcined at 450°C for 2 h, exhibited an overpotential of 430 mV at a current density of 10 mA·cm −2 in 0.1 M KOH, a Tafel slope of 93.69 mV·dec −1 , and a C dl of 242.75 mF·cm −2 . Upon exceeding 450°C during calcination, the gradual expulsion of heteroatoms from the matrix resulted in structural destruction. Consequently, the electrocatalytic activity of the sample decreased because of the gradual removal of surface oxygen vacancy concentration and Co 3+ /Co 3+ + Co 2+ . The methodology employed in this study not only efficiently recovers Ni 2+ and Co 2+ from the NSL but also prepares electrocatalysts with superior performance for the oxygen evolution reaction.
研究领域:
材料科学
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环境工程
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电化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Chaowu Wang,Qibo Zhang
Efficiently recovering critical metals from secondary resources is crucial to decreasing the environmental impact of mineral-resource mining and reducing production costs and process energy consumption. Herein, we propose a simple and comprehensive approach to recycle Co 3 O 4 from waste choline chloride/ethylene glycol (named Ethaline) electrolyte containing Co(II) ions along with solvent regeneration. Through the rational coordination adjustment using water, [CoCl 4 ] 2− complex in the Ethaline-based electrolyte is transformed to [CoCl 2 (H 2 O) 4 ] 0 and [CoCl 2 (H 2 O) 5 ] + to facilitate precipitation separation. Adding oxalic acid (OA) as a precipitator can reach 97.1% cobalt recovery efficiency with a high value-added Co 3 O 4 rod-like structure obtained by calcining the oxalate precipitate. In addition, the water-containing solvent can be regenerated via reduced pressure distillation with a high recovery efficiency of up to 98.0%. FT-IR and 1 H NMR characterizations verify that the regenerated Ethaline exhibits good structural stability. Impressively, the proposed recovery path shows high recovery efficiencies for both cobalt and Ethaline in various practical Co(II) ion-containing electrolytes. This study establishes a novel technical pathway for the resource utilization of metal-bearing waste Ethaline electrolytes, which shows an excellent prospect in solvent recycling after metal processing.
研究领域:
材料科学
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环境工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ao Zhou,Dan Zhang,Zhihong Liu,Zhiyong Liu
With the retirement of rechargeable lithium-ion batteries (LIBs) entering peak period, the recycling of LiCoO 2 has become a hot topic. The spent LiCoO 2 batteries are rich in carcinogenic metal Co and high-value metal Li, so they are needed to be recovered in time before causing serious environmental pollution and resource waste. Thus, a clean and efficient process is proposed for the comprehensive recovery of Li, Co, and Mn from the spent LiCoO 2 cathode material. It is an integrated pyro-hydrometallurgical process, mainly consisting of sulfation roasting with NH 4 HSO 4 and selective sulfurizing leaching with (NH 4 ) 2 S solution. Using low melting point ammonium salt as roasting auxiliary, 99.7 %, 99.1 %, and 99.8 % of Li, Co, and Mn in the spent LiCoO 2 powder can be converted into sulfate when roasting under 400 ℃ for 75 min. Then 99.5 % of Li in the sulfation roasting product can be selectively leached with an aqueous (NH 4 ) 2 S solution, which is also a precipitator for Co, Mn, and impurity Al. In addition, 96.4 % of Co and 96.0 % of Mn in the sulfurized precipitate can be separated with impurity elements Al and C via oxidation roasting–water leaching process. Compared to traditional recycling, this method can achieve a higher Li leaching rate at a low roasting temperature, and the recovery of Co and Mn can be realized without adding any acid/base reagents or impurity cations. More importantly, the circulation of NH 3 /NH 4 + and S element in the recycling system has been taken into account, making it an environmental-friendly and economical process. In this study, the sulfation reduction roasting and selective sulfurizing leaching mechanisms were both revealed in details, and the behavior of the valuable elements was also elucidated.
研究领域:
环境科学
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冶金工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
·
IF 7.2
Yu Wang,Yanjuan Zhang,Caixia Lv,Guangye Wei,Long Meng,Jiajie Fu,Zhihui Yu,Jingkui Qu
Due to the complex process, environmental impact, and high cost of conventional solvent extraction for Ni and Co recovery from mixed hydroxide precipitate, this study introduces an ammonia leaching process to selectively extract Ni and Co. Specifically, a ball milling and water washing pretreatment removes soluble Mg 2+ , followed by (NH 4 ) 2 CO 3 leaching, which dissolves 98 % Ni and 96 % Co, leaving impurities (Mn, Mg, Fe, Al) unreactive. The leachate contains 25.68 g/L of Ni, 2.4 g/L of Co, and 0.07 g/L of Mn, with Mg, Fe, and Al levels below detection limits, demonstrating effective separation of Ni and Co. Mn is also removed through ammonia leaching and subsequent precipitation as MnCO 3 . Kinetic analysis revealed that the diffusion-controlled process allows for efficient extraction at lower temperatures, further reducing energy consumption. Moreover, the ammonia solution can be reused for five consecutive cycles, maintaining leaching efficiencies above 95 % for Ni and 92 % for Co, offering cost savings. This method simplifies the recovery process, eliminates the need for organic solvents, reduces environmental impact, and lowers operational costs, making it a more sustainable and economically viable alternative for industrial applications.
研究领域:
冶金工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2025
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IF 6.3
Xin Liu,Ruixue Hu,Shiran Zhu,Xiangyu Liu,Yu Fang,Yihang Li,Wei Wei
Background The demand for adsorption technologies that facilitate the recovery and upcycling of the valuable metallic element, Co, has been increasing. The recovery of Co from wastewater using metal–organic frameworks (MOFs), which are promising adsorbents, is considerably limited because of the lack of selective adsorption sites. Furthermore, research on the upcycling of Co remains inadequate. Methods Herein, we develop an integrated strategy combining ion imprinting modification and photodeposition for the selective recovery and upcycling of divalent Co ions (Co(II)) using MOF adsorbents. Significant findings First, Co ion–imprinted sites are constructed on a typical MOF adsorbent, MIL-125 (labeled CoIP-ML), via molecular engineering using glycylglycine. Compared with the original aminated MIL-125, CoIP-ML exhibits a superior performance, achieving the maximum adsorption capacity ( q m = 218.6 mg/g) and selectivity (selective coefficient k Co(II)/Ni(II) = 3.61) for Co(II) via the chelation of Schiff base groups and adsorption at terminal carboxyl groups. The Co(II) adsorbed on CoIP-ML is upcycled through a facile photodeposition process into Co oxides, which function as a Fenton-like catalyst. The optimal catalyst effectively activates peroxymonosulfate for the removal of chloroquine diphosphate and chlortetracycline hydrochloride, achieving the upcycling of Co(II). This study presents a unique MOF-functionalization paradigm.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）