The high compacted density LiNi<sub>0.5-x</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>Mg<sub>x</sub>O<sub>2</sub> cathode material for lithium-ion batteries was syn...The high compacted density LiNi<sub>0.5-x</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>Mg<sub>x</sub>O<sub>2</sub> cathode material for lithium-ion batteries was synthesized by high temperature solid-state method, taking the Mg element as a doping element and the spherical Ni<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub> (OH)<sub>2</sub>, Li<sub>2</sub>CO<sub>3</sub> as raw materials. The effects of calcination temperature on the structure and properties of the products were investigated. The structure and morphology of cathode materials powder were analyzed by X-ray diffraction spectroscopy (XRD) and scanning electronmicroscopy (SEM). The electrochemical properties of the cathode materials were studied by charge-discharge test and cyclic properties test. The results show that LiNi<sub>0.4985</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub> Mg<sub>0.0015</sub>O<sub>2</sub> cathode material prepared at calcination temperature 930°C has a good layered structure, and the compacted density of the electrode sheet is above 3.68 g/cm<sup>3</sup>. The discharge capacity retention rate is more than 97.5% after 100 cycles at a charge-discharge rate of 1C, displaying a good cyclic performance.展开更多
Li/Ni mixing negatively influences the discharge capacity of lithium nickel oxide and high-nickel ternary cathode materials.However,accurately measuring the Li/Ni mixing degree is difficult due to the preferred orient...Li/Ni mixing negatively influences the discharge capacity of lithium nickel oxide and high-nickel ternary cathode materials.However,accurately measuring the Li/Ni mixing degree is difficult due to the preferred orientation of labbased XRD measurements using Bragg–Brentano geometry.Here,we find that employing spherical harmonics in Rietveld refinement to eliminate the preferred orientation can significantly decrease the measurement error of the Li/Ni mixing ratio.The Li/Ni mixing ratio obtained from Rietveld refinement with spherical harmonics shows a strong correlation with discharge capacity,which means the electrochemical capacity of lithium nickel oxide and high-nickel ternary cathode can be estimated by the Li/Ni mixing degree.Our findings provide a simple and accurate method to estimate the Li/Ni mixing degree,which is valuable to the structural analysis and screening of the synthesis conditions of lithium nickel oxide and high-nickel ternary cathode materials.展开更多
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
An adequate wide temperature electrolyte for high nickel ternary cathode is urgent to further develop high energy density batteries.Herein,a comprehensive double-salt local high-concentration sulfolane-based electroly...An adequate wide temperature electrolyte for high nickel ternary cathode is urgent to further develop high energy density batteries.Herein,a comprehensive double-salt local high-concentration sulfolane-based electrolyte(DLi)is proposed with specific sheath structure to build stable interface on the LiNi_(0.8)Co_(0.1)Mn_(0.1O2)(NCM811)cathode at wide operating temperature between−60 and 55℃.Lithium perchlorate(LiClO_(4))in combination with high concentration lithium bis-(trifluoromethanesulfonyl)imide(LiTFSI)strengthens the internal interaction between anion and cation in the solvation structure,increasing Li+transference number of the electrolyte to 0.61.Moreover,the structure and component characteristics of the passive interface layer on NCM811 are modulated,decreasing desolvation energy of Li+ions,benefiting Li+transport dynamics especially at low temperature,and also ensuring the interfacial stability at a wide operating temperature range.As a result,the cathode with DLi exhibits excellent high-temperature storage performance and high capacity retention of 80.5%in 100 cycles at 55℃.Meanwhile,the Li||NCM811 cells can deliver high discharge capacity of 160.1,136.1,and 110.3 mAh·g^(−1)under current density of 0.1 C at−20,−40,and−60℃,maintaining 84.5%,71.8%,and 58.2%of the discharge capacity at 30℃,respectively.Moreover,it enables NCM811 cathode to achieve a reversible capacity of 142.8 mAh·g^(−1)in 200 cycles at−20℃and 0.2 C.Our studies shed light on the molecular strategy of wide operational temperature electrolyte for high nickel ternary cathode.展开更多
文摘The high compacted density LiNi<sub>0.5-x</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub>Mg<sub>x</sub>O<sub>2</sub> cathode material for lithium-ion batteries was synthesized by high temperature solid-state method, taking the Mg element as a doping element and the spherical Ni<sub>0.5</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub> (OH)<sub>2</sub>, Li<sub>2</sub>CO<sub>3</sub> as raw materials. The effects of calcination temperature on the structure and properties of the products were investigated. The structure and morphology of cathode materials powder were analyzed by X-ray diffraction spectroscopy (XRD) and scanning electronmicroscopy (SEM). The electrochemical properties of the cathode materials were studied by charge-discharge test and cyclic properties test. The results show that LiNi<sub>0.4985</sub>Co<sub>0.2</sub>Mn<sub>0.3</sub> Mg<sub>0.0015</sub>O<sub>2</sub> cathode material prepared at calcination temperature 930°C has a good layered structure, and the compacted density of the electrode sheet is above 3.68 g/cm<sup>3</sup>. The discharge capacity retention rate is more than 97.5% after 100 cycles at a charge-discharge rate of 1C, displaying a good cyclic performance.
基金Project supported by the Natural Science Foundation of Beijing(Grant No.Z200013)the Beijing Municipal Science&Technology(Grant No.Z191100004719001)the National Natural Science Foundation of China(Grant Nos.52325207 and 22005333)。
文摘Li/Ni mixing negatively influences the discharge capacity of lithium nickel oxide and high-nickel ternary cathode materials.However,accurately measuring the Li/Ni mixing degree is difficult due to the preferred orientation of labbased XRD measurements using Bragg–Brentano geometry.Here,we find that employing spherical harmonics in Rietveld refinement to eliminate the preferred orientation can significantly decrease the measurement error of the Li/Ni mixing ratio.The Li/Ni mixing ratio obtained from Rietveld refinement with spherical harmonics shows a strong correlation with discharge capacity,which means the electrochemical capacity of lithium nickel oxide and high-nickel ternary cathode can be estimated by the Li/Ni mixing degree.Our findings provide a simple and accurate method to estimate the Li/Ni mixing degree,which is valuable to the structural analysis and screening of the synthesis conditions of lithium nickel oxide and high-nickel ternary cathode materials.
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supported by the National Natural Science Foundation of China(Nos.52172180 and 51872026)the National Key R&D Program of China(No.2018YFB0104300).
文摘An adequate wide temperature electrolyte for high nickel ternary cathode is urgent to further develop high energy density batteries.Herein,a comprehensive double-salt local high-concentration sulfolane-based electrolyte(DLi)is proposed with specific sheath structure to build stable interface on the LiNi_(0.8)Co_(0.1)Mn_(0.1O2)(NCM811)cathode at wide operating temperature between−60 and 55℃.Lithium perchlorate(LiClO_(4))in combination with high concentration lithium bis-(trifluoromethanesulfonyl)imide(LiTFSI)strengthens the internal interaction between anion and cation in the solvation structure,increasing Li+transference number of the electrolyte to 0.61.Moreover,the structure and component characteristics of the passive interface layer on NCM811 are modulated,decreasing desolvation energy of Li+ions,benefiting Li+transport dynamics especially at low temperature,and also ensuring the interfacial stability at a wide operating temperature range.As a result,the cathode with DLi exhibits excellent high-temperature storage performance and high capacity retention of 80.5%in 100 cycles at 55℃.Meanwhile,the Li||NCM811 cells can deliver high discharge capacity of 160.1,136.1,and 110.3 mAh·g^(−1)under current density of 0.1 C at−20,−40,and−60℃,maintaining 84.5%,71.8%,and 58.2%of the discharge capacity at 30℃,respectively.Moreover,it enables NCM811 cathode to achieve a reversible capacity of 142.8 mAh·g^(−1)in 200 cycles at−20℃and 0.2 C.Our studies shed light on the molecular strategy of wide operational temperature electrolyte for high nickel ternary cathode.