Electro-chemo-mechanical analysis of the effect of bending deformation on the interface of flexible solid-state battery

Flexible solid-state battery has several unique characteristics including high flexibility,easy portability,and high safety,which may have broad application prospects in new technology products such as rollup displays,power implantable medical devices,and wearable equipments.The interfacial mechanical and electrochemical problems caused by bending deformation,resulting in the battery damage and failure,are particularly interesting.Herein,a fully coupled electro-chemo-mechanical model is developed based on the actual solid-state battery structure.Concentration-dependent material parameters,stress-dependent diffusion,and potential shift are considered.According to four bending forms(k=8/mm,0/mm,-8/mm,and free),the results show that the negative curvature bending is beneficial to reducing the plastic strain during charging/discharging,while the positive curvature is detrimental.However,with respect to the electrochemical performance,the negative curvature bending creates a negative potential shift,which causes the battery to reach the cut-off voltage earlier and results in capacity loss.These results enlighten us that suitable electrode materials and charging strategy can be tailored to reduce plastic deformation and improve battery capacity for different forms of battery bending.

Unconventional dislocation starvation behavior of medium-entropy alloy single crystal pillars containing pre-existing dislocations

The excellent dislocation storage ability of bulk multi-principal element alloys(MPEAs)has been widely reported.To date,however,the underlying mechanisms of dislocation escape behavior in small-size facecentered cubic(FCC)MPEAs have rarely been studied.Here,we quantitatively control the initial dislocation densities(-10^(15) m^(-2) and -10^(16) m^(-2))by large-scale molecular dynamics(MD)simulations and perform uniaxial compression simulations to compare the dislocation starvation behavior of CrCoNi with pure Cu single crystal pillars(SCPs).The analysis reveals that the CrCoNi SCPs with low initial dislocation density(-10^(15) m^(-2))can continuously accommodate mobile dislocations,and the critical dimension for dislocation starvation is about 30 nm.In particular,the CrCoNi SCPs with chemical short-range ordering(SRO)exhibit better dislocation storage and multiplication abilities than the random solid solution(RSS)samples even when the initial dislocation density is low.However,the presence of a large number of pre-existing dislocation locks governs the strong dislocation multiplication ability of the small-size RSS CrCoNi SCPs,in obvious contrast to the deformation of all pure Cu SCPs which is completely dominated by intermittent mobile dislocation starvation.Most importantly,we reveal the fundamental physics for the good dislocation storage of CrCoNi SCPs at small sizes from the perspective of chemical heterogeneity.The new phenomena reported in this work provide a unique atomic-scale perspective for understanding the microscopic physical origin of the mechanical behavior of MPEAs and the discovery of extremely slow dislocation escape behavior in small-scaled pillars,providing a reliable basis for the development of the dislocation starvation model.

Novel Zr-doped β-Li_(3)PS_(4) solid electrolyte for all-solid-state lithium batteries with a combined experimental and computational approach

All-solid-state lithium batteries(ASSLBs)are promising for safety and high-energy-density large-scale energy storage.In this contribution,we propose a Li_(3–4x)Zr_(x)PS_(4)(LZPS)by Zr-dopedβ-Li_(3)PS_(4)(LPS)as a novel solid electrolyte(SE)for ASSLBs based on experimental and simulation methods.The structure,electronic property,mechanical property,and ionic transport properties of LZPS(x=0,0.03,0.06,and 0.1)are investigated with first-principles calculations.Meanwhile,LZPS is prepared by solid states reaction method.By combining experimental analysis and first-principles calculations,it is confirmed that a small amount of Zr4+can be successfully doped into the framework ofβ-LPS composites without significantly compromising structural integrity.When the Zr^(4+)concentration is x=0.03,the doped material Li_(2.88)Zr_(0.03)PS_(4)exhibits the highest ionic conductivity(5.1×10^(−4)S·cm^(−1))at 30℃,and the Li-ion migration energy barrier is the lowest.The Li_(2.88)Zr_(0.03)PS_(4)SE has obtained the best mechanical properties,the good ductility,and shear deformation resistance,which can better maintain the structural stability of the battery.In addition,the Li/Li symmetrical cell is assembled,which shows excellent electrochemical stability of electrolyte against lithium.The constructed all-solid-state batteries(LiCoO_(2)-Li_(6)PS_(5)Cl|Li_(2.88)Zr_(0.03)PS_(4)|Li-In)delivers an initial discharge capacity of 130.4 mAh·g^(−1)at 0.2 C and a capacity retention of 85.1%after 100 cycles at room temperature.This study provides a promising electrolyte for the application of ASSLBs with high ionic conductivity and excellent stability against lithium.