The recycling of spent lithium-ion batteries(LIBs) is crucial for environmental protection and resource sustainability.However,the economic recovery of spent LIBs remains challenging due to low Li recovery efficiency ...The recycling of spent lithium-ion batteries(LIBs) is crucial for environmental protection and resource sustainability.However,the economic recovery of spent LIBs remains challenging due to low Li recovery efficiency and the need for multiple separation operations.Here,we propose a process involving mixed HCl-H_(2)SO_(4) leaching-spray pyrolysis for recycling spent ternary LIBs,achieving both selective Li recovery and the preparation of a ternary oxide precursor.Specifically,the process transforms spent ternary cathode(LiNi_(x)Co_yMn_(2)O_(2),NCM) powder into Li_(2)SO_(4) solution and ternary oxide,which can be directly used for synthesizing battery-grade Li_(2)CO_(3) and NCM cathode,respectively.Notably,SO_(4)^(2-) selectively precipitates with Li^(+) to form thermostable Li_(2)SO_(4) during the spray pyrolysis,which substantially improves the Li recovery efficiency by inhibiting Li evaporation and intercalation.Besides,SO_(2) emissions are avoided by controlling the molar ratio of Li^(+)/SO_(4)^(2-)(≥2:1),The mechanism of the preferential formation of Li_(2)SO_(4) is interpreted from its reverse solubility variation with temperature.During the recycling of spent NCM811,92% of Li is selectively recovered,and the regenerated NCM811 exhibits excellent cycling stability with a capacity retention of 81.7% after 300 cycles at 1 C.This work offers a simple and robust process for the recycling of spent NCM cathodes.展开更多
Micro-electrolysis(ME)technology is investigated for improving the efficiency of removal of pentavalent antimony(Sb(V))from the environment.In this study,an ME system composed of scrap iron filings,waste manganese fil...Micro-electrolysis(ME)technology is investigated for improving the efficiency of removal of pentavalent antimony(Sb(V))from the environment.In this study,an ME system composed of scrap iron filings,waste manganese fillings,and activated carbon(Fe-Mn-C ME)was used to efficiently remove Sb(V).The results proved that,compared with conventional iron-carbon micro-electrolysis(Fe-C ME),Fe-Mn-C ME significantly enhances the removal rate of Sb(V)when the hydraulic retention time is 10–24 h.The Fe-Mn flocs produced by this system were analyzed using X-ray diffraction(XRD),energy-dispersive X-ray spectroscopy(EDS),X-ray photoelectron spectroscopy(XPS),and Brunauer-Emmett-Teller(BET)surface area analysis,which revealed that the flocs were mostly Mn-substituted FeOOH and had a relatively larger specific surface area,providing better adsorption performance.Furthermore,it was found that the removal rate of Sb(V)decreased as the iron-carbon mass ratio increased,while it first increased and then decreased as the manganese content increased.The reduction of Fe(III)was accelerated with an increase in the addition of manganese,leading to an increase in the concentration of Fe(II).The electron transfer and the formation of Fe(II)were facilitated by the potential difference between manganese and carbon,as well as by the formation of microcells between iron and manganese,which improved the reduction ability of Sb(V).From our thorough investigation and research,this is the first report that has proposed Fe-Mn-C ME for removing antimony.It provides a novel approach and technological support for removing Sb(V)efficiently.展开更多
Localized high-concentration electrolytes(LHCE) have shown good compatibility with high-voltage lithium(Li)-metal batteries, but their practicality is yet to be proved in terms of cost and safety. Here we develop a hy...Localized high-concentration electrolytes(LHCE) have shown good compatibility with high-voltage lithium(Li)-metal batteries, but their practicality is yet to be proved in terms of cost and safety. Here we develop a hybrid-LHCE with favorable integrated properties by combining the merits of two representative diluents, fluorobenzene(FB) and 1,1,2,2-tetrafluoroethyl-2,2,2-trifluoroethyl ether(TFE). Specifically,the extremely cheap and lightweight FB significantly reduces the cost and density of electrolyte, while the fire-retardant TFE circumvents the flammable nature of FB and thus greatly improves the safety of electrolyte. Moreover, the FB–TFE mixture enhances the thermodynamic stability of hybrid-LHCE and renders a controllable defluorination of FB, contributing to the formation of a thin and durable inorganic-rich solid electrolyte interphase(SEI) with rapid ion-transport kinetics. Benefiting from the designed hybridLHCE, a Li|NCM523 battery demonstrates excellent cycling performance(215 cycles, 91% capacity retention) under challenging conditions of thin Li-anode(30 μm) and high cathode loading(3.5 m Ah/cm^(2)).展开更多
UV/H2O2 and UV/peroxodisulfate （PDS） processes were adopted to degrade a typical β-blocker atenolol （ATL）. The degradation efficiencies under various operational parameters （oxidant dosage, pH, HCO3-, humic acid...UV/H2O2 and UV/peroxodisulfate （PDS） processes were adopted to degrade a typical β-blocker atenolol （ATL）. The degradation efficiencies under various operational parameters （oxidant dosage, pH, HCO3-, humic acid （HA）, NO3- , and Cl-） were compared. Principal factor analysis was also performed with a statistical method for the two processes. It was found that increasing the specific dosage of the two peroxides （[peroxide]0/[ATL]0 ） ranging from 1：1 to 8：1 led to a faster degradation rate but also higher peroxide residual. Within the pH range 3-11, the optimum pH was 7 for the UV/PDS process and elevating pH benefitted the UV/H 2O2 process. The presence of HCO3- , HA, and Cl adversely affected ATL oxidation in both processes. The NO3- concentration 1-3 mmol/L accelerated the destruction of ATL by the UV/PDS process, but further increase of NO3- concentration retarded the degradation process, contrary to the case in the UV/H2O2 process. The rank orders of effects caused by the six operational parameters were pH ≈ specific dosage 〉 [HA]0 〉 [NO3-]0 〉 [HCO3-]0 〉 [Cl-]0 for the UV/H2O2 process and specific dosage 〉 pH 〉 [HA]0 〉 [NO3-]0 〉 [HCO3-]0 〉[Cl-]0 for the UV/PDS process. The UV/PDS process was more sensitive to changes in operational parameters than the UV/H2O2 process but more efficient in ATL removal under the same conditions.展开更多
基金Fund of University of South China (201RGC013 and 200XQD052)。
文摘The recycling of spent lithium-ion batteries(LIBs) is crucial for environmental protection and resource sustainability.However,the economic recovery of spent LIBs remains challenging due to low Li recovery efficiency and the need for multiple separation operations.Here,we propose a process involving mixed HCl-H_(2)SO_(4) leaching-spray pyrolysis for recycling spent ternary LIBs,achieving both selective Li recovery and the preparation of a ternary oxide precursor.Specifically,the process transforms spent ternary cathode(LiNi_(x)Co_yMn_(2)O_(2),NCM) powder into Li_(2)SO_(4) solution and ternary oxide,which can be directly used for synthesizing battery-grade Li_(2)CO_(3) and NCM cathode,respectively.Notably,SO_(4)^(2-) selectively precipitates with Li^(+) to form thermostable Li_(2)SO_(4) during the spray pyrolysis,which substantially improves the Li recovery efficiency by inhibiting Li evaporation and intercalation.Besides,SO_(2) emissions are avoided by controlling the molar ratio of Li^(+)/SO_(4)^(2-)(≥2:1),The mechanism of the preferential formation of Li_(2)SO_(4) is interpreted from its reverse solubility variation with temperature.During the recycling of spent NCM811,92% of Li is selectively recovered,and the regenerated NCM811 exhibits excellent cycling stability with a capacity retention of 81.7% after 300 cycles at 1 C.This work offers a simple and robust process for the recycling of spent NCM cathodes.
基金supported by the National Key R&D Program of China(No.2019YFC0408400)the National Natural Science Foundation of China(No.51878597).
文摘Micro-electrolysis(ME)technology is investigated for improving the efficiency of removal of pentavalent antimony(Sb(V))from the environment.In this study,an ME system composed of scrap iron filings,waste manganese fillings,and activated carbon(Fe-Mn-C ME)was used to efficiently remove Sb(V).The results proved that,compared with conventional iron-carbon micro-electrolysis(Fe-C ME),Fe-Mn-C ME significantly enhances the removal rate of Sb(V)when the hydraulic retention time is 10–24 h.The Fe-Mn flocs produced by this system were analyzed using X-ray diffraction(XRD),energy-dispersive X-ray spectroscopy(EDS),X-ray photoelectron spectroscopy(XPS),and Brunauer-Emmett-Teller(BET)surface area analysis,which revealed that the flocs were mostly Mn-substituted FeOOH and had a relatively larger specific surface area,providing better adsorption performance.Furthermore,it was found that the removal rate of Sb(V)decreased as the iron-carbon mass ratio increased,while it first increased and then decreased as the manganese content increased.The reduction of Fe(III)was accelerated with an increase in the addition of manganese,leading to an increase in the concentration of Fe(II).The electron transfer and the formation of Fe(II)were facilitated by the potential difference between manganese and carbon,as well as by the formation of microcells between iron and manganese,which improved the reduction ability of Sb(V).From our thorough investigation and research,this is the first report that has proposed Fe-Mn-C ME for removing antimony.It provides a novel approach and technological support for removing Sb(V)efficiently.
基金supported by the National Natural Science Foundation of China (No. 21808125)China Postdoctoral Science Foundation (No. 2020M672805)supported by Tsinghua National Laboratory for Information Science and Technology。
文摘Localized high-concentration electrolytes(LHCE) have shown good compatibility with high-voltage lithium(Li)-metal batteries, but their practicality is yet to be proved in terms of cost and safety. Here we develop a hybrid-LHCE with favorable integrated properties by combining the merits of two representative diluents, fluorobenzene(FB) and 1,1,2,2-tetrafluoroethyl-2,2,2-trifluoroethyl ether(TFE). Specifically,the extremely cheap and lightweight FB significantly reduces the cost and density of electrolyte, while the fire-retardant TFE circumvents the flammable nature of FB and thus greatly improves the safety of electrolyte. Moreover, the FB–TFE mixture enhances the thermodynamic stability of hybrid-LHCE and renders a controllable defluorination of FB, contributing to the formation of a thin and durable inorganic-rich solid electrolyte interphase(SEI) with rapid ion-transport kinetics. Benefiting from the designed hybridLHCE, a Li|NCM523 battery demonstrates excellent cycling performance(215 cycles, 91% capacity retention) under challenging conditions of thin Li-anode(30 μm) and high cathode loading(3.5 m Ah/cm^(2)).
文摘UV/H2O2 and UV/peroxodisulfate （PDS） processes were adopted to degrade a typical β-blocker atenolol （ATL）. The degradation efficiencies under various operational parameters （oxidant dosage, pH, HCO3-, humic acid （HA）, NO3- , and Cl-） were compared. Principal factor analysis was also performed with a statistical method for the two processes. It was found that increasing the specific dosage of the two peroxides （[peroxide]0/[ATL]0 ） ranging from 1：1 to 8：1 led to a faster degradation rate but also higher peroxide residual. Within the pH range 3-11, the optimum pH was 7 for the UV/PDS process and elevating pH benefitted the UV/H 2O2 process. The presence of HCO3- , HA, and Cl adversely affected ATL oxidation in both processes. The NO3- concentration 1-3 mmol/L accelerated the destruction of ATL by the UV/PDS process, but further increase of NO3- concentration retarded the degradation process, contrary to the case in the UV/H2O2 process. The rank orders of effects caused by the six operational parameters were pH ≈ specific dosage 〉 [HA]0 〉 [NO3-]0 〉 [HCO3-]0 〉 [Cl-]0 for the UV/H2O2 process and specific dosage 〉 pH 〉 [HA]0 〉 [NO3-]0 〉 [HCO3-]0 〉[Cl-]0 for the UV/PDS process. The UV/PDS process was more sensitive to changes in operational parameters than the UV/H2O2 process but more efficient in ATL removal under the same conditions.
