A closed-loop process for recycling LiNi_xCo_yMn_((1-x-y))O_2 from mixed cathode materials of lithium-ion batteries

With the rapid development of consumer electronics and electric vehicles(EV), a large number of spent lithium-ion batteries(LIBs) have been generated worldwide. Thus, effective recycling technologies to recapture a significant amount of valuable metals contained in spent LIBs are highly desirable to prevent the environmental pollution and resource depletion. In this work, a novel recycling technology to regenerate a LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2 cathode material from spent LIBs with different cathode chemistries has been developed. By dismantling, crushing,leaching and impurity removing, the LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2(selected as an example of LiNi_xCo_yMn_(1-x-y)O_2) powder can be directly prepared from the purified leaching solution via co-precipitation followed by solid-state synthesis. For comparison purposes, a fresh-synthesized sample with the same composition has also been prepared using the commercial raw materials via the same method. X-ray diffraction(XRD), scanning electron microscopy(SEM) and electrochemical measurements have been carried out to characterize these samples. The electrochemical test result suggests that the re-synthesized sample delivers cycle performance and low rate capability which are comparable to those of the freshsynthesized sample. This novel recycling technique can be of great value to the regeneration of a pure and marketable LiNi_xCo_yMn_(1-x-y)O_2 cathode material with low secondary pollution.

The origins of kinetics hysteresis and irreversibility of monoclinic Li_(3)V_(2)(PO_(4))_(3)

Monoclinic Li_(2)V_(2)(PO_(4))_(3);is a promising cathode material with complex charge–discharge behavior.Previous structural investigation of this compound mainly focuses on local environments;while the reaction kinetics and the driving force of irreversibility of this material remain unclear.To fully understand the above issues,both the equilibrium and the non-equilibrium reaction routes have been systematically investigated in this study.Multiple characterization techniques including X-ray diffraction,variable temperature(spinning rate)and ex/in situ ^(7)Li,^(31)P solid state NMR have been employed to provide comprehensive insights into kinetics,dynamics,framework structure evolution and charge ordering,which is essential to better design and application of lithium transition metal phosphate cathodes.Our results suggest that the kinetics process between the non-equilibrium and the quasi-equilibrium delithiation pathways from Li_(2)V_(2)(PO_(4))_(3);to V_(2)(PO_(4))_(3);is related with a slow relaxation from two-site to one-site delithiation.More importantly,it has been demonstrated that the irreversibility in this system is not solely affected by cation and/or charge ordering/disordering,but mainly driven by framework structure distortion.

Structural evolution of layered oxide cathodes for spent Li-ion batteries:Degradation mechanism and repair strategy

Sustainable development has long been recognized as one of the most critical issues in today’s energy and environment-conscious society.It has never been more urgent to recycle and reuse the end-of-life cathode materials.Here,this work systematically investigates the structure-critical degradation mechanism of polycrystalline LiNi_(x)Co_(y)Mn_(1−x−y)O_(2)(NCM),combining experimental characterization and DFT simulations.Targeting the key degradation factors,a synergistic repair strategy based on deep mechanochemical activation and heat treatment was successfully proposed to direct regenerate the degradedNCMmaterial.Studies indicate the induction and promotion of synergistic repair technique on the reconstruction of particlemorphology,the recovery of the chemical composition and crystal structure,and the favorable transformation of the impurities phase in the failed materials.In particular,the synergistic repair process induces a gradient distribution of LiF and further enables partial fluorine doping into the NCM surface,forming abundant oxygen vacancies and increasing the content of highly reactive Ni2+.Benefiting from the comprehensive treatment for the multi-scale and multi-form degradation behaviors,the repaired material exhibits a capacity of 176.8 mA h g^(-1)at 0.1 C,which is comparable to the corresponding commercial material(172.8 mA h g^(-1)).The satisfactory capacity of the recovered cathode proves that it is an effective direct renovating strategy.

Performance simulation method and state of health estimation for lithium-ion batteries based on aging-effect coupling model

Accurate simulation of characteristics performance and state of health(SOH)estimation for lithium-ion batteries are critical for battery management systems(BMS)in electric vehicles.Battery simplified electrochemical model(SEM)can achieve accurate estimation of battery terminal voltage with less computing resources.To ensure the applica-bility of life-cycle usage,degradation physics need to be involved in SEM models.This work conducts deep analysis on battery degradation physics and develops an aging-effect coupling model based on an existing improved single particle(ISP)model.Firstly,three mechanisms of solid electrolyte interface(SEI)film growth throughout life cycle are analyzed,and an SEI film growth model of lithium-ion battery is built coupled with the ISP model.Then,a series of identification conditions for individual cells are designed to non-destructively determine model parameters.Finally,battery aging experiment is designed to validate the battery performance simulation method and SOH estimation method.The validation results under different aging rates indicate that this method can accurately es-timate characteristics performance and SOH for lithium-ion batteries during the whole life cycle.