Oxidative exfoliation of spent cathode carbon:A two-in-one strategy for its decontamination and high-valued application

Spent cathode carbon(SCC)from aluminum electrolysis is a potential graphite resource.However,full use of the SCC remains a challenge,since it contains many hazardous substances(e.g.,fluoride salts,cyanides),encapsulated within the thick carbon layers and thus posing serious environmental concerns.This work presents a chemical oxidative exfoliation route to achieve the recycling of SCC and the decontaminated SCC with high-valued graphene oxide(GO)-like carbon structures(SCC-GO)is applied as an excellent adsorbent for organic pollutants.Specifically,after the oxidative exfoliation,the embedded hazardous constituents are fully exposed,facilitating their subsequent removal by aqueous leaching.Moreover,benefiting from the enhanced specific surface areas along with abundant O-containing functional groups,the as-produced SCC-GO,shows an adsorption capacity as high as 347 mg·g^(-1)when considering methylene blue as a pollutant model,which exceeds most of the recently reported carbon-based adsorbents.Our study provides a feasible solution for the efficient recycling of hazardous carbonaceous wastes.

A Sustainable Strategy for Spent Cathode Carbon Blocks Hazardous Waste Recycling Using Binary Molten Salt Thermal Treatment

Waste-to-Energy treatment is a promising path to environment and energy management in the future.This work detailed a binary molten salt thermal treatment methodology for the detoxification of spent cathode carbon block(SCCB)waste and the recycling of carbonaceous materials.The thermal behavior of SCCB and SCCB blended with molten salts was investigated.It was found that the NaCl-Na_(2)CO_(3)binary molten salts significantly contributed to reducing pyrolysis onset temperature by 334.3 K compared to that of SCCB itself(i.e.,activation energy of pyrolysis reaction was reduced from 4.24×10^(5)to 2.30×10^(5)J/mol),thus helping to lower thermal treatment energy consumption.With the addition of binary molten salts,the residue after thermal treatment in a horizontal tube furnace experiment was separated into two layers.The bottom-layer residue was mainly composed of molten salts.The fluorine content in the form of NaF and CaF_(2)of top-layer residue was reduced significantly while the carbon content remained unchanged.Specifically,the leaching concentration of fluoride ion was decreased from 4620 mg/L to 856 mg/L.It is noted that the NaF and CaF_(2)can be removed through water-leaching and hydrothermal acid-leaching methods and thus the carbonaceous materials with a calorific value of 17.5 MJ/kg were obtained.

Preferentially selective extraction of lithium from spent LiCoO_(2)cathodes by medium-temperature carbon reduction roasting

Lithium recovery from spent lithium-ion batteries(LIBs)have attracted extensive attention due to the skyrocketing price of lithium.The medium-temperature carbon reduction roasting was proposed to preferential selective extraction of lithium from spent Li-CoO_(2)(LCO)cathodes to overcome the incomplete recovery and loss of lithium during the recycling process.The LCO layered structure was destroyed and lithium was completely converted into water-soluble Li2CO_(3)under a suitable temperature to control the reduced state of the cobalt oxide.The Co metal agglomerates generated during medium-temperature carbon reduction roasting were broken by wet grinding and ultrasonic crushing to release the entrained lithium.The results showed that 99.10%of the whole lithium could be recovered as Li2CO_(3)with a purity of 99.55%.This work provided a new perspective on the preferentially selective extraction of lithium from spent lithium batteries.

Preparation of lithium-ion battery anode materials from graphitized spent carbon cathode derived from aluminum electrolysis

Graphitized spent carbon cathode(SCC)is a hazardous solid waste generated in the aluminum electrolysis process.In this study,a flotation-acid leaching process is proposed for the purification of graphitized SCC,and the use of the purified SCC as an anode material for lithium-ion batteries is explored.The flotation and acid leaching processes were separately optimized through one-way experiments.The maximum SCC carbon content(93wt%)was achieved at a 90%proportion of−200-mesh flotation particle size,a slurry concentration of 10wt%,a rotation speed of 1600 r/min,and an inflatable capacity of 0.2 m^(3)/h(referred to as FSCC).In the subsequent acid leaching process,the SCC carbon content reached 99.58wt%at a leaching concentration of 5 mol/L,a leaching time of 100 min,a leaching temperature of 85°C,and an HCl/FSCC volume ratio of 5:1.The purified graphitized SCC(referred to as FSCC-CL)was utilized as an anode material,and it exhibited an initial capacity of 348.2 mAh/g at 0.1 C and a reversible capacity of 347.8 mAh/g after 100 cycles.Moreover,compared with commercial graphite,FSCC-CL exhibited better reversibility and cycle stability.Thus,purified SCC is an important candidate for anode material,and the flotation-acid leaching purification method is suitable for the resourceful recycling of SCC.

An environmentally benign and sustainable process for carbon recovery and efficient defluorination of spent carbon cathode

A systematic and green low-temperature sulfation roasting−water leaching strategy was put forward to achieve a very high fluorine removal rate of 97.82%for spent carbon cathode(SCC),which was believed as a hazardous solid waste.And the carbon could be recycled with a purity of 90.29 wt.%in the flaky microstructure.Thermodynamic analysis and the results of SEM,XRD and EDS indicate that most of the fluoride could convert into water-soluble sulfate at low temperature.And the highest fluorine removal rate could be obtained when<0.15 mm SCC particles were mixed with sulfuric acid at a liquid-to-solid ratio of 1:1,and then roasted at 300℃ for 0.5 h.The sulfate was removed to purify the carbon via water-leaching process.Avrami exponents and corresponding activation energy for the roasting and leaching process demonstrated that both processes are controlled by diffusion.

Waste to wealth:Defect-rich Ni-incorporated spent LiFePO_(4)for efficient oxygen evolution reaction

The development of efficient strategies to recycle lithium-ion battery(LIB)electrode materials is an important yet challenging goal for the sustainable management of battery waste.This work reports a facile and economically efficient method to convert spent cathode material,LiFePO_(4),into a high-performance NiFe oxy/hydroxide catalyst for the oxygen evolution reaction(OER).Herein,Ni-LiFePO_(4)is synthesized via the wetness impregnation method and further evolves into defect-rich NiFe oxy/hydroxide nanosheets during the OER.The introduction of the Ni promoter together with in situ evolution strengthens the electronic interactions among the metal sites and creates an abundance of defects.Experimentally,the evolved Ni-LiFePO_(4)delivers a low overpotential of 285 mV at 10 mA cm-^(2)and a small Tafel slope of 45 mV dec^(-1),outperforming pristine LiFePO_(4)and is even superior to the benchmark catalyst RuO_(2).Density functional theory(DFT)calculations reveal that the introduction of Ni effectively activates Fe sites by optimizing the free energy of the*OOH intermediate and that the abundance of oxygen defects facilitates the oxygen desorption step,synergistically enhancing the OER performance of LiFePO_(4).As a green and versatile method,this is a new opportunity for the scalable fabrication of excellent electrocatalysts based on spent cathode materials.