Regeneration of Al-doped LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) cathode material by simulated hydrometallurgy leachate of spent lithium-ion batteries

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.

Review of the electrochemical performance and interfacial issues of high-nickel layered cathodes in inorganic all-solid-state batteries

All-solid-state batteries potentially exhibit high specific energy and high safety,which is one of the development directions for nextgeneration lithium-ion batteries.The compatibility of all-solid composite electrodes with high-nickel layered cathodes and inorganic solid electrolytes is one of the important problems to be solved.In addition,the interface and mechanical problems of high-nickel layered cathodes and inorganic solid electrolyte composite electrodes have not been thoroughly addressed.In this paper,the possible interface and mechanical problems in the preparation of high-nickel layered cathodes and inorganic solid electrolytes and their interface reaction during charge–discharge and cycling are reviewed.The mechanical contact problems from phenomena to internal causes are also analyzed.Uniform contact between the high-nickel cathode and solid electrolyte in space and the ionic conductivity of the solid electrolyte are the prerequisites for the good performance of a high-nickel layered cathode.The interface reaction and contact loss between the high-nickel layered cathode and solid electrolyte in the composite electrode directly affect the passage of ions and electrons into the active material.The buffer layer constructed on the high-nickel cathode surface can prevent direct contact between the active material and electrolyte and slow down their interface reaction.An appropriate protective layer can also slow down the interface contact loss by reducing the volume change of the high-nickel layered cathode during charge and discharge.Finally,the following recommendations are put forward to realize the development vision of high-nickel layered cathodes:(1)develop electrochemical systems for high-nickel layered cathodes and inorganic solid electrolytes;(2)elucidate the basic science of interface and electrode processes between high-nickel layered cathodes and inorganic solid electrolytes,clarify the mechanisms of the interfacial chemical and electrochemical reactions between the two materials,and address the intrinsic safety issues;(3)strengthen the development of research and engineering technologies and their preparation methods for composite electrodes with high-nickel layered cathodes and solid electrolytes and promote the industrialization of all-solid-state batteries.

Stabilizing effects of atomic Ti doping on high-voltage high-nickel layered oxide cathode for lithium-ion rechargeable batteries

High-voltage high-nickel lithium layered oxide cathodes show great application prospects to meet the ever-increasing demand for further improvement of the energy density of rechargeable lithium-ion batteries(LIBs)mainly due to their high output capacity.However,severe bulk structural degradation and undesired electrode-electrolyte interface reactions seriously endanger the cycle life and safety of the battery.Here,2 mol%Ti atom is used as modified material doping into LiNi_(0.8)Co_(0.2)Mn_(0.2O2)(NCM)to reform LiNi_(0.6)Co_(0.2)Mn_(0.18)Ti_(0.02)O_(2)(NCM-Ti)and address the long-standing inherent problem.At a high cut-off voltage of 4.5 V,NCM-Ti delivers a higher capacity retention ratio(91.8%vs.82.9%)after 150 cycles and a superior rate capacity(118 vs.105 mAh·g^(-1))at the high current density of 10 C than the pristine NCM.The designed high-voltage full battery with graphite as anode and NCM-Ti as cathode also exhibits high energy density(240 Wh·kg^(-1))and excellent electrochemical performance.The superior electrochemical behavior can be attributed to the improved stability of the bulk structure and the electrode-electrolyte interface owing to the strong Ti-O bond and no unpaired electrons.The in-situ X-ray diffraction analysis demonstrates that Ti-doping inhibits the undesired H2-H3 phase transition,minimizing the mechanical degradation.The ex-situ TEM and X-ray photoelectron spectroscopy reveal that Ti-doping suppresses the release of interfacial oxygen,reducing undesired interfacial reactions.This work provides a valuable strategic guideline for the application of high-voltage high-nickel cathodes in LIBs.

Porous ternary complex metal oxide nanoparticles converted from core/shell nanoparticles

We demonstrate an easy and scalable low-temperature process to convert porous ternary complex metal oxide nanoparticles from solution-synthesized core^shell metal oxide nanopartides by thermal annealing. The final products demonstrate superior electrochemical properties with a large capacity and high stability during fast charging/discharging cycles for potential applications as advanced lithium-ion battery （LIB） electrode materials. In addition, a new breakdown mechanism was observed on these novel electrode materials.

Ternary Metal–Organic Framework Derived 2D Fe_(2)O_(3)/Co_(3)O_(4)/NiO/NC Heterostructured Nanosheets for Super Lithium Storage

Fe_(2)O_(3)/Co_(3)O_(4)/NiO/NC nanosheets have been successfully prepared via a two-step annealing process of ternary metal coordination polymer. Attributing to the synergistic effects of the multiple metal oxides and the unique 2D nanosheet structure, the improved electrical conductivity and effective electron/ion transfer enables Fe_(2)O_(3)/Co_(3)O_(4)/NiO/NC electrode to exhibit excellent electrochemical properties with outstanding rate capacity and cycling stability. This work may pave the way to construct ternary metal oxide electrode material with an excellent electrochemical performance by introducing multiple metal oxides.

Self-template formation of porous yolk-shell structure Mo-doped NiCo2O4 toward enhanced lithium storage performance as anode material

Hollow ternary metal oxides have shown enormous potential in lithium-ion batteries(LIBs),which is ascribed to their complex chemical composition,abundant active defect sites,and the synergy effect be-tween metals.In this work,we synthesized Mo-doped NiCo_(2)O_(4) porous spheres with yolk-shell structure by using a simple self-templating method.Surprisingly,other than the yolk-shell structure we had ob-tained,the inner core of the yolk-shell was also porous,which could fully enhance the electrolyte infil-tration and promote the transmission of lithium ions(Li+)and electrons(e−).The diameter of the porous core in the yolk-shell sphere was about 530 nm,and the outer shell’s thickness was up to 110 nm.In addition,the unique pores in the core appeared in the diameter of about 85 nm.With this structure,the volume expansion of the anode could be well inhibited during charge/discharge.It exhibited prominent electrochemical performance with high reversible capacity(1338 mA h g^(−1) at 100 mA g^(−1)),satisfactory cycle life(1360 mA h g^(−1) after 200 cycles at 100 mA g^(−1)),and exceptional rate capability(820 mA h g^(−1) at 2000 mA g^(−1))as anode material in LIBs.

Boosting the electrochemical performance of LiNi_(0.6)Mn_(0.2)Co_(0.2)O_2 through a trace amount of Mg-B co-doping

The extended cycle life of cells is often sacrificed at the expense of high specific energy for high-nickel materials.Cation doping is a promising method to build high-nickel cathode with high energy density and long cycle life.Herein,a trace amount of Mg-B co-doping in LiNi_(0.6)Mn_(0.2)Co_(0.2)O_2(NMC622)is investigated in this work,which shows improved structural and electrochemical stability of 1%Mg-0.5%B co-doped material at both 30 and 55℃in coin-cell.Comprehensive chemical composition,structural,and surface analysis are carried out in this paper.It was found that all the selected materials have a similar composition to the target.Moreover,Mg and B doping have different effects on the crystal structural change of NMC622,to be more specific,the c-lattice parameter increases with Mg doping,while the Li^(+)/Ni^(2+)mixing content increases when B was incorporated into the lattice.Furthermore,the microstructure of primary particles was changed by B doping significantly as confirmed by the SEM images.There were marginal benefits in terms of structural and electrochemical stability of materials introduced by Mg or B sole doping.In comparison,incorporating a suitable amount of both Mg and B into NMC622,we found the capacity retention of cells was noticeably improved by reducing the impedance growth and preventing cation mixing during cycling.This study demonstrates the importance of co-incorporation of Mg,B,and optimizing the co-dopant content to stabilize NMC622 as cathode for lithium-ion batteries.