A uniform Al-doped LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) cathode material was prepared using a coprecipitation method to take advantage of the positive effect of Al on regenerated NCM(Ni,Co,Mn)cathode materials and ameliora...A uniform Al-doped LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) cathode material was prepared using a coprecipitation method to take advantage of the positive effect of Al on regenerated NCM(Ni,Co,Mn)cathode materials and ameliorate cumbersome and high-cost impurity removal processes during lithium-ion battery recycling.When the Al^(3+) content in the leachate was 1 at.%with respect to the total amount of transition metals(Ni,Co,and Mn),the produced Al-doped NCM cathode material increased concentrations of lattice oxygen and Ni^(2+).The initial specific capacity at 0.1C was 167.4 mA·h/g,with a capacity retention of 79.1%after 400 cycles at 1C.Further,this Al-doped sample showed improved rate performance and a smaller electrochemical impedance.These findings provide a reference for developing industrial processes to resynthesize cathode materials with improved electrochemical performance by incorporating Al^(3+) impurities produced during lithium-ion battery recycling.展开更多
To effectively separate and recover Co(Ⅱ) from the leachate of spent lithium-ion battery cathodes,we investigated solvent extraction with quaternary ammonium salt N263 in the sodium nitrite system.NO_(2)^(-)combines ...To effectively separate and recover Co(Ⅱ) from the leachate of spent lithium-ion battery cathodes,we investigated solvent extraction with quaternary ammonium salt N263 in the sodium nitrite system.NO_(2)^(-)combines with Co(Ⅱ) to form an anion [Co(NO_(2))_(3)]^(-),and it is then extracted by N263.The extraction of Co(Ⅱ) is related to the concentration of NO_(2)^(-).The extraction efficiency of Co(Ⅱ) reaches the maximum of99.16%,while the extraction efficiencies of Ni(Ⅱ),Mn(Ⅱ),and Li(Ⅰ) are 9.27%-9.80% under the following conditions:30vol% of N263 and15vol% of iso-propyl alcohol in sulfonated kerosene,the volume ratio of the aqueous-to-organic phase is 2:1,the extraction time is 30 min,and1 M sodium nitrite in 0.1 MHNO_(3).The theoretical stages require for the Co(Ⅱ) extraction are performed in the McCabe–Thiele diagram,and the extraction efficiency of Co(Ⅱ) reaches more than 99.00% after three-stage counter-current extraction with Co(Ⅱ) concentration of 2544mg/L.When the HCl concentration is 1.5 M,the volume ratio of the aqueous-to-organic phase is 1:1,the back-extraction efficiency of Co(Ⅱ)achieves 91.41%.After five extraction and back-extraction cycles,the Co(Ⅱ) extraction efficiency can still reach 93.89%.The Co(Ⅱ) extraction efficiency in the actual leaching solution reaches 100%.展开更多
The recycling of graphite from spent lithium-ion batteries(LIBs)is overlooked due to its relatively low added value and the lack of efficient recovering methods.To reuse the spent graphite anodes,we need to eliminate ...The recycling of graphite from spent lithium-ion batteries(LIBs)is overlooked due to its relatively low added value and the lack of efficient recovering methods.To reuse the spent graphite anodes,we need to eliminate their useless components(mainly the degraded solid electrolyte interphase,SEI)and reconstruct their damaged structure.Herein,a facile and efficient strategy is proposed to recycle the spent graphite on the basis of the careful investigation of the composition of the cycled graphite anodes and the rational design of the regeneration processes.The regenerated graphite,which is revitalized by calcination treatment and acid leaching,delivers superb rate performance and a high specific capacity of 370 mAh g^(-1)(~99% of its theoretical capacity)after 100 cycles at 0.1 C,superior to the commercial graphite anodes.The improved electrochemical performance could be attributed to unchoked Li^(+) transport channels and enhanced charge transfer reaction due to the effective destruction of the degraded SEI and the full recovery of the damaged structure of the spent graphite.This work clarifies that the electrochemical performance of the regenerated graphite could be deteriorated by even a trace amount of the residual“impurity”and provides a facile method for the efficient regeneration of graphite anodes.展开更多
Along with the extensive application of energy storage devices,the spent lithium-ion batteries(LIBs)are unquestionably classified into the secondary resources due to its high content of several valuable metals.However...Along with the extensive application of energy storage devices,the spent lithium-ion batteries(LIBs)are unquestionably classified into the secondary resources due to its high content of several valuable metals.However,current recycling methods have the main drawback to their tedious process,especially the purification and separation process.Herein,we propose a simplified process to recycle both cathode(LiCoO_(2))and anode(graphite)in the spent LIBs and regenerate newly high-performance anode material,CoO/CoFe2O4/expanded graphite(EG).This process not only has the advantages of succinct procedure and easy control of reaction conditions,but also effectively separates and recycles lithium from transition metals.The 98.43%of lithium is recovered from leachate when the solid product CoO/CoFe2O4/EG is synthesized as anode material for LIBs.And the product exhibits improved cyclic stability(890 mAh g^(-1) at 1 A g^(-1) after 700 cycles)and superior rate capability(208 mAh g^(-1) at 5 A g^(-1)).The merit of this delicate recycling design can be summarized as three aspects:the utilization of Fe impurity in waste LiCoO_(2),the transformation of waste graphite to EG,and the regeneration of anode material.This approach properly recycles the valuable components of spent LIBs,which introduces an insight into the future recycling.展开更多
基金supported by Anhui Province Research and Development Innovation Project for Automotive Power Battery Efficient Recycling System, China
文摘A uniform Al-doped LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) cathode material was prepared using a coprecipitation method to take advantage of the positive effect of Al on regenerated NCM(Ni,Co,Mn)cathode materials and ameliorate cumbersome and high-cost impurity removal processes during lithium-ion battery recycling.When the Al^(3+) content in the leachate was 1 at.%with respect to the total amount of transition metals(Ni,Co,and Mn),the produced Al-doped NCM cathode material increased concentrations of lattice oxygen and Ni^(2+).The initial specific capacity at 0.1C was 167.4 mA·h/g,with a capacity retention of 79.1%after 400 cycles at 1C.Further,this Al-doped sample showed improved rate performance and a smaller electrochemical impedance.These findings provide a reference for developing industrial processes to resynthesize cathode materials with improved electrochemical performance by incorporating Al^(3+) impurities produced during lithium-ion battery recycling.
基金financially supported by the National Natural Science Foundation of China(No.51804084)the Natural Science Foundation of Guangxi Province,China(No.2021GXNSFAA220096)the Science and Technology Major Project of Guangxi Province,China(No.AA17204100)。
文摘To effectively separate and recover Co(Ⅱ) from the leachate of spent lithium-ion battery cathodes,we investigated solvent extraction with quaternary ammonium salt N263 in the sodium nitrite system.NO_(2)^(-)combines with Co(Ⅱ) to form an anion [Co(NO_(2))_(3)]^(-),and it is then extracted by N263.The extraction of Co(Ⅱ) is related to the concentration of NO_(2)^(-).The extraction efficiency of Co(Ⅱ) reaches the maximum of99.16%,while the extraction efficiencies of Ni(Ⅱ),Mn(Ⅱ),and Li(Ⅰ) are 9.27%-9.80% under the following conditions:30vol% of N263 and15vol% of iso-propyl alcohol in sulfonated kerosene,the volume ratio of the aqueous-to-organic phase is 2:1,the extraction time is 30 min,and1 M sodium nitrite in 0.1 MHNO_(3).The theoretical stages require for the Co(Ⅱ) extraction are performed in the McCabe–Thiele diagram,and the extraction efficiency of Co(Ⅱ) reaches more than 99.00% after three-stage counter-current extraction with Co(Ⅱ) concentration of 2544mg/L.When the HCl concentration is 1.5 M,the volume ratio of the aqueous-to-organic phase is 1:1,the back-extraction efficiency of Co(Ⅱ)achieves 91.41%.After five extraction and back-extraction cycles,the Co(Ⅱ) extraction efficiency can still reach 93.89%.The Co(Ⅱ) extraction efficiency in the actual leaching solution reaches 100%.
基金supported by the National Key R&D Program of China(2021YFB2400300)Key R&D Program of Hubei Province of China(2020BAB088)+2 种基金National Natural Science Foundation of China(52002277)the Fundamental Research Funds for the Central Universities(2021GCRC001)Guangdong Basic and Applied Basic Reuter Foundation(2021A1515011748).
文摘The recycling of graphite from spent lithium-ion batteries(LIBs)is overlooked due to its relatively low added value and the lack of efficient recovering methods.To reuse the spent graphite anodes,we need to eliminate their useless components(mainly the degraded solid electrolyte interphase,SEI)and reconstruct their damaged structure.Herein,a facile and efficient strategy is proposed to recycle the spent graphite on the basis of the careful investigation of the composition of the cycled graphite anodes and the rational design of the regeneration processes.The regenerated graphite,which is revitalized by calcination treatment and acid leaching,delivers superb rate performance and a high specific capacity of 370 mAh g^(-1)(~99% of its theoretical capacity)after 100 cycles at 0.1 C,superior to the commercial graphite anodes.The improved electrochemical performance could be attributed to unchoked Li^(+) transport channels and enhanced charge transfer reaction due to the effective destruction of the degraded SEI and the full recovery of the damaged structure of the spent graphite.This work clarifies that the electrochemical performance of the regenerated graphite could be deteriorated by even a trace amount of the residual“impurity”and provides a facile method for the efficient regeneration of graphite anodes.
基金This work was supported by National Natural Science Foundation of China(51902347,51822812,51772334,51778627).
文摘Along with the extensive application of energy storage devices,the spent lithium-ion batteries(LIBs)are unquestionably classified into the secondary resources due to its high content of several valuable metals.However,current recycling methods have the main drawback to their tedious process,especially the purification and separation process.Herein,we propose a simplified process to recycle both cathode(LiCoO_(2))and anode(graphite)in the spent LIBs and regenerate newly high-performance anode material,CoO/CoFe2O4/expanded graphite(EG).This process not only has the advantages of succinct procedure and easy control of reaction conditions,but also effectively separates and recycles lithium from transition metals.The 98.43%of lithium is recovered from leachate when the solid product CoO/CoFe2O4/EG is synthesized as anode material for LIBs.And the product exhibits improved cyclic stability(890 mAh g^(-1) at 1 A g^(-1) after 700 cycles)and superior rate capability(208 mAh g^(-1) at 5 A g^(-1)).The merit of this delicate recycling design can be summarized as three aspects:the utilization of Fe impurity in waste LiCoO_(2),the transformation of waste graphite to EG,and the regeneration of anode material.This approach properly recycles the valuable components of spent LIBs,which introduces an insight into the future recycling.
