Elucidating the suppression of lithium dendrite growth with a void-reduced anti-perovskite solid-state electrolyte pellet for stable lithium metal anodes

Solid-state lithium-metal batteries,with their high theoretical energy density and safety,are highly promising as a next-generation battery contender.Among the alternatives proposed as solid-state electrolyte,lithium-rich anti-perovskite(Li RAP)materials have drawn the most interest because of high theoretical Li^(+)conductivity,low cost and easy processing.Although solid-state electrolytes are believed to have the potential to physically inhibit the lithium dendrite growth,lithium-metal batteries still suffer from the lithium dendrite growth and thereafter the short circuiting.The voids in practical Li RAP pellets are considered as the root cause.Herein,we show that reducing the voids can effectively suppress the lithium dendrite growth.The voids in the pellet resulted in an irregular Li^(+)flux distribution and a poor interfacial contact with lithium metal anode;and hence the ununiform lithium dendrites.Consequently,the lithium-metal symmetric cell with void-reduced Li_(2)OHCl-HT pellet was able to display excellent cycling performance(750 h at 0.4 m A cm^(-2))and stability at high current density(0.8 m A cm^(-2)for 120 h).This study provides not only experimental evidence for the impact of the voids in Li RAP pellets on the lithium dendrite growth,but also a rational pellet fabrication approach to suppress the lithium dendrite growth.

Synthesis and Conductivity Characterization of Anti-Perovskite Na3OX Solid Electrolytes for All Solid Na-Ion Batteries

Solid electrolytes for all solid sodium-ion batteries have been attracting much attention as an alternative energy storage system, which have the advantage of being extremely safe because it can be charged quickly and is nonflammable. We have synthesized anti-perovskite type Na3OX (X = Br, and I) electrolytes with high purity, by reactions of halogen mixtures with sodium oxides. After mixing, it was filled in an alumina crucible and heated for 6 hours at 330°C. It was confirmed that a large crystal strain was introduced by eutectication, which might reduce the activation energy of Na ion conduction and lead to an improvement of the conductivity. A relatively higher ionic conductivity of σ = 1.55 × 10-7 S/cm at 60°C has been obtained for Na3OBr0.6I0.4, which is about three orders higher than that in literature. A different ratio of X (X = Br, I) ions was added into sodium oxide to make the Na3OX crystal. The influence of strain introduction on optimizing the bottleneck and improving the conductivity was discussed.

Transparent glassy composites incorporating lead-free anti-perovskite halide nanocrystals enable tunable emission and ultrastable X-ray imaging

Lead halide perovskite materials exhibit excellent scintillation performance,which,however,suffer from serious stability and toxicity problems.In contrast,the heavy metal-free anti-perovskite materials[MX_(4)]XA_(3)(A=alkali metal;M=transition metal;X=Cl,Br,I),a class of electron-inverted perovskite derivatives,exhibit robust structural and photophysical stability.Here,we design and prepare a lead-free[MnBr_(4)]BrCs_(3) anti-perovskite nanocrystal(NC)-embedded glass for efficient X-ray-excited luminescence with high-resolution X-ray imaging with a spatial resolution of 19.1 Ip mm^(-1).Due to the unique crystal structure and the protection of the glass matrix,the Cs_(3)MnBr_(5) NC-embedded glass exhibits excellent X-ray irradiation stability,thermal stability,and water resistance.These merits enable the demonstration of real-time and durable X-ray radiography based on the developed glassy composite.This work could stimulate the research and development of novel metal halide anti-perovskite materials and open a new path for future development in the field of high-resolution and ultrastable X-ray imaging.

Structure inversion asymmetry enhanced electronic structure and electrical transport in 2D A3SnO(A=Ca,Sr,and Ba)antiperovskite monolayers

Anti-perovskites A3SnO(A=Ca,Sr,and Ba)are an important class of materials due to the emergence of Dirac cones and tiny mass gaps in their band structures originating from an intricate interplay of crystal symmetry,spin–orbit coupling,and band overlap.This provides an exciting playground for modulating their electronic properties in the two-dimensional(2D)limit.Herein,we employ first-principles density functional theory(DFT)calculations by combining dispersion-corrected SCAN+rVV10 and mBJ functionals for a comprehensive side-by-side comparison of the structural,thermodynamic,dynamical,mechanical,electronic,and thermoelectric properties of bulk and monolayer(one unit cell thick)A3SnO anti-perovskites.Our results show that 2D monolayers derived from bulk A3SnO anti-perovskites are structurally and energetically stable.Moreover,Rashba-type splitting in the electronic structure of Ca3SnO and Sr3SnO monolayers is observed owing to strong spin–orbit coupling and inversion asymmetry.On the other hand,monolayer Ba3SnO exhibits Dirac cone at the high-symmetryΓpoint due to the domination of band overlap.Based on the predicted electronic transport properties,it is shown that inversion asymmetry plays an essential character such that the monolayers Ca3SnO and Sr3SnO outperform thermoelectric performance of their bulk counterparts.

Enhancement of–OH content on mechanical properties of antiperovskite solid electrolytes

All-solid-state batteries,renowned for their enhanced safety and high energy density,have garnered broad interest.Oxide solid electrolytes are highly anticipated for their balanced performance.However,their high Young’s modulus and inadaptability to volume change during cycling lead to poor contact and eventual battery failure.In this work,Young’s modulus of Li_(1+x)(OH)_(x)Cl samples is lowered to a level comparable to that of sulfide by regulating the–OH content.As the–OH content increases,Young’s modulus of Li_(1+x)(OH)_(x)Cl samples decreases significantly.This may be due to the local aggregation of–OH groups,forming cavities similar to LiOH structure,which reduces the bonding of the structure.On the premise of high Li-ion conductivity and electrochemical stability,the lowered Young’s modulus improves the contact between the solid electrolyte and the electrodes,forming a strong and stable interfacial layer,thereby improving interfacial and cycling stability.The symmetrical lithium metal cell shows excellent cycle performance of 600 h,and the assembled LiFePO_(4)|Li_(2.4)(OH)1.4Cl|Li cell shows significantly enhanced cycling endurance with 80%capacity retention after 150 cycles.This work not only emphasizes the crucial importance of Young’s modulus in improving interface issues but also offers innovative approaches to advance the mechanical properties of solid electrolytes.