Lithium-ion batteries(LIBs)that reached their end-of-life(EoL)require recycling,rather than disposal,to recirculate valuable metals and protect the environment.This led us to investigate the extraction of metals from ...Lithium-ion batteries(LIBs)that reached their end-of-life(EoL)require recycling,rather than disposal,to recirculate valuable metals and protect the environment.This led us to investigate the extraction of metals from the cathodes of EoL lithium-titanate batteries using ethylenediaminetetraacetic acid disodium(EDTA-2Na).In this work,an orthogonal array was used to design experiments and sig-nal-to-noise calculations were used to define the optimal conditions,which were 0.50 mol/L EDTA-2Na,pH=6,75℃,180 min,2%pulp density,and 300 r/min,resulting in 97.96%,94.79%,96.45%,and 98.89%leaching efficiencies for Li,Ni,Co,and Mn,respectively.Stat-istically significant interactions between variables were then identified using Pearson’s correlation at the 95%confidence interval,and the pH and temperature were found to be significant.The extraction efficiency decreased as the pH increased,but increased as the temperat-ure increased.Machine learning fitting using linear regression for multi-output prediction was unsatisfactory,whereas random forest re-gression(RFR)produced satisfactory results.Permutation importance was computed on the fitted RFR to determine feature importance,and confirmed that the pH and temperature were influential variables;however,the time and pulp density were also noted.As the fitted RFR failed to satisfactorily predict leaching efficiencies in additional validation experiments,we recommend increasing the number of ex-periments and using additional fitting models.An additional analysis that included the initial oxidation-reduction potential(optimal 33.3 mV)revealed this to be the most important variable,the effect of which largely overshadows those of all the other variables.Finally,an environmental assessment highlighted the benefits of the chelating extraction;however,the economic assessment indicated room for improvement.展开更多
Resistive switching devices with a high self-rectifying ratio are important for achieving the crossbar memristor array that overcomes the sneak current issue.Herein,we demonstrate a single amorphous lithium lanthanum ...Resistive switching devices with a high self-rectifying ratio are important for achieving the crossbar memristor array that overcomes the sneak current issue.Herein,we demonstrate a single amorphous lithium lanthanum titanium oxide(LLTO)layer based Pt/LLTO/Pt device possessing a self-rectifying ratio higher than 1 × 10^(4) that is comparable to the reported devices with complicated multi-layer stacking structures.Moreover,the device shows forming-free and highly uniform bipolar resistive switching(BRS)characteristic that facilitates the potential applications.The trap-controlled and trap-free space charge limited conductions are demonstrated to dominate the high and low resistance states of the device,respectively.The fast migration of lithium ions under external voltage accelerates the electron injection across the Pt/LLTO interface and also the space charge accumulation in the LLTO layer,and as a result,the high performance of the Pt/LLTO/Pt device was achieved.As demonstrated Pt/LLTO/Pt device sheds a light on the potential applications of the lithium ionic conductors in self-rectifying resistive switching devices.展开更多
Lithium ion sieve(LIS)has attracted great attention due to its high adsorption selectivity towards Li+.Herein,a new type of Zr-doped Ti-LIS(HZrTO)was synthesized by a simple calcination method.The adsorption capacity ...Lithium ion sieve(LIS)has attracted great attention due to its high adsorption selectivity towards Li+.Herein,a new type of Zr-doped Ti-LIS(HZrTO)was synthesized by a simple calcination method.The adsorption capacity increased from 56.3 mgg-1(before doping)to 93.2 mgg-1 after doping in LiOH solution(lithium 1.8gL-1).The adsorption isotherm and adsorption kinetics of HZrTO accord with the Langmuir isotherm and the pseudo-second-order kinetic equation,respectively.Batch experiments showed that HZrTO has good stability and selectivity.In addition,HZrTO was granulated via epoxy resin(E-12),and the obtained granular adsorbent showed good adsorption capacity,excellent stability and high selectivity towards Li+.展开更多
Through meticulous design, a Li-lacking Cr2O5 cathode is physically mixed with Li-rich Li（1.2）Ni（0.13）Co（0.13）Mn（0.54）O2（LNCM） cathode to form composite cathodes LNCM@x Cr2O5（x = 0, 0.1, 0.2, 0.3, 0.35, 0.4...Through meticulous design, a Li-lacking Cr2O5 cathode is physically mixed with Li-rich Li（1.2）Ni（0.13）Co（0.13）Mn（0.54）O2（LNCM） cathode to form composite cathodes LNCM@x Cr2O5（x = 0, 0.1, 0.2, 0.3, 0.35, 0.4, mass ratio） in order to make use of the excess lithium produced by the Li-rich component in the first charge-discharge process. The initial coulombic efficiency（ICE） of LNCM half-cell has been significantly increased from75.5%（x = 0） to 108.9%（x = 0.35）. A novel full-cell comprising LNCM@Cr2O5composite cathode and Li4Ti5O（12） anode has been developed. Such electrode accordance, i.e., LNCM@Cr2O5//Li4Ti5O（12）（＂L-cell＂）, shows a particularly high ICE of97.7%. The ＂L-cell＂ can transmit an outstanding reversible capacity up to 250 mA h g-1and has 94% capacity retention during 50 cycles. It also has superior rate capacities as high as122 and 94 mA h g-（-1）at 1.25 and 2.5 A g-（-1）current densities,which are even better in comparison of Li-rich//graphite fullcell（＂G-cell＂）. The high performance of ＂L-cell＂ benefiting from the well-designed coulombic efficiency accordance mechanism displays a great potential for fast charge-discharge applications in future high-energy lithium ion batteries.展开更多
Flexible portable electronic devices have attracted increasing attention during the last decade. Energy consumption of such devices is ever increasing and performing power sources, that are moreover flexible, need to ...Flexible portable electronic devices have attracted increasing attention during the last decade. Energy consumption of such devices is ever increasing and performing power sources, that are moreover flexible, need to be developed to seamlessly integrate into such architectures. While lithium-ion batteries appear to be the best solution to meet the power and energy requirements, their structural and mechanical considerations still need to be addressed. Here, we realize and study the impact on the electrochemical performances of carbon nanotubes （CNTs） based, current collector-free and binder-free, Li-ion battery electrodes. Multi-walled carbon nanotubes acting as a mechanical and electron conductive scaffold enable structural flexibility and good electrochemical performances. Flexible Li-ion cells made with such electrodes show promising performances while being realized through simple manu- facturing approaches.展开更多
基金supported by the National Research Foundation of Korea(NRF)grants funded by the Korea government(MSIT)(Nos.RS-2024-00406500 and RS-2024-00458682).
文摘Lithium-ion batteries(LIBs)that reached their end-of-life(EoL)require recycling,rather than disposal,to recirculate valuable metals and protect the environment.This led us to investigate the extraction of metals from the cathodes of EoL lithium-titanate batteries using ethylenediaminetetraacetic acid disodium(EDTA-2Na).In this work,an orthogonal array was used to design experiments and sig-nal-to-noise calculations were used to define the optimal conditions,which were 0.50 mol/L EDTA-2Na,pH=6,75℃,180 min,2%pulp density,and 300 r/min,resulting in 97.96%,94.79%,96.45%,and 98.89%leaching efficiencies for Li,Ni,Co,and Mn,respectively.Stat-istically significant interactions between variables were then identified using Pearson’s correlation at the 95%confidence interval,and the pH and temperature were found to be significant.The extraction efficiency decreased as the pH increased,but increased as the temperat-ure increased.Machine learning fitting using linear regression for multi-output prediction was unsatisfactory,whereas random forest re-gression(RFR)produced satisfactory results.Permutation importance was computed on the fitted RFR to determine feature importance,and confirmed that the pH and temperature were influential variables;however,the time and pulp density were also noted.As the fitted RFR failed to satisfactorily predict leaching efficiencies in additional validation experiments,we recommend increasing the number of ex-periments and using additional fitting models.An additional analysis that included the initial oxidation-reduction potential(optimal 33.3 mV)revealed this to be the most important variable,the effect of which largely overshadows those of all the other variables.Finally,an environmental assessment highlighted the benefits of the chelating extraction;however,the economic assessment indicated room for improvement.
基金supported by the National Key Research and Development Program of China(No.2019YFB2005801)the National Natural Science Foundation of China(Nos.52061135205,51731003,51971024,51971023,51971027,51927802)the Beijing Natural Science Foundation Key Program(No.Z190007)。
文摘Resistive switching devices with a high self-rectifying ratio are important for achieving the crossbar memristor array that overcomes the sneak current issue.Herein,we demonstrate a single amorphous lithium lanthanum titanium oxide(LLTO)layer based Pt/LLTO/Pt device possessing a self-rectifying ratio higher than 1 × 10^(4) that is comparable to the reported devices with complicated multi-layer stacking structures.Moreover,the device shows forming-free and highly uniform bipolar resistive switching(BRS)characteristic that facilitates the potential applications.The trap-controlled and trap-free space charge limited conductions are demonstrated to dominate the high and low resistance states of the device,respectively.The fast migration of lithium ions under external voltage accelerates the electron injection across the Pt/LLTO interface and also the space charge accumulation in the LLTO layer,and as a result,the high performance of the Pt/LLTO/Pt device was achieved.As demonstrated Pt/LLTO/Pt device sheds a light on the potential applications of the lithium ionic conductors in self-rectifying resistive switching devices.
基金supported by National Natural Science Foundation of China(grant Nos.21676291 and 22005191)Natural Science Foundation of Shanghai(grant No.18ZR1427800)+1 种基金“111”Innovation and Talent Recruitment Base on Photochemical and Energy Materials(grant No.D18020)Shanghai Engineering Research Center of Green Energy Chemical Engineering(grant No.18DZ2254200).
文摘Lithium ion sieve(LIS)has attracted great attention due to its high adsorption selectivity towards Li+.Herein,a new type of Zr-doped Ti-LIS(HZrTO)was synthesized by a simple calcination method.The adsorption capacity increased from 56.3 mgg-1(before doping)to 93.2 mgg-1 after doping in LiOH solution(lithium 1.8gL-1).The adsorption isotherm and adsorption kinetics of HZrTO accord with the Langmuir isotherm and the pseudo-second-order kinetic equation,respectively.Batch experiments showed that HZrTO has good stability and selectivity.In addition,HZrTO was granulated via epoxy resin(E-12),and the obtained granular adsorbent showed good adsorption capacity,excellent stability and high selectivity towards Li+.
基金supported by the National Natural Science Foundation of China(51577175)NSAF(U1630106)
文摘Through meticulous design, a Li-lacking Cr2O5 cathode is physically mixed with Li-rich Li（1.2）Ni（0.13）Co（0.13）Mn（0.54）O2（LNCM） cathode to form composite cathodes LNCM@x Cr2O5（x = 0, 0.1, 0.2, 0.3, 0.35, 0.4, mass ratio） in order to make use of the excess lithium produced by the Li-rich component in the first charge-discharge process. The initial coulombic efficiency（ICE） of LNCM half-cell has been significantly increased from75.5%（x = 0） to 108.9%（x = 0.35）. A novel full-cell comprising LNCM@Cr2O5composite cathode and Li4Ti5O（12） anode has been developed. Such electrode accordance, i.e., LNCM@Cr2O5//Li4Ti5O（12）（＂L-cell＂）, shows a particularly high ICE of97.7%. The ＂L-cell＂ can transmit an outstanding reversible capacity up to 250 mA h g-1and has 94% capacity retention during 50 cycles. It also has superior rate capacities as high as122 and 94 mA h g-（-1）at 1.25 and 2.5 A g-（-1）current densities,which are even better in comparison of Li-rich//graphite fullcell（＂G-cell＂）. The high performance of ＂L-cell＂ benefiting from the well-designed coulombic efficiency accordance mechanism displays a great potential for fast charge-discharge applications in future high-energy lithium ion batteries.
文摘Flexible portable electronic devices have attracted increasing attention during the last decade. Energy consumption of such devices is ever increasing and performing power sources, that are moreover flexible, need to be developed to seamlessly integrate into such architectures. While lithium-ion batteries appear to be the best solution to meet the power and energy requirements, their structural and mechanical considerations still need to be addressed. Here, we realize and study the impact on the electrochemical performances of carbon nanotubes （CNTs） based, current collector-free and binder-free, Li-ion battery electrodes. Multi-walled carbon nanotubes acting as a mechanical and electron conductive scaffold enable structural flexibility and good electrochemical performances. Flexible Li-ion cells made with such electrodes show promising performances while being realized through simple manu- facturing approaches.
