One-step calcination synthesis of interface-coherent crystallized and surface-passivated LiNi_(0.5)Mn_(1.5)O_(4) for high-voltage lithium-ion battery

LiNi_(0.5)Mn_(1.5)O_(4)(LNMO)with a spinel crystal structure presents a compelling avenue towards the development of economic cobalt-free and high voltage(~5 V)lithium-ion batteries.Nevertheless,the elevated operational voltage of LNMO gives rise to pronounced interfacial interactions between the distorted surface lattices characterized by Jahn-Teller(J-T)distortions and the electrolyte constituents.Herein,a localized crystallized coherent LaNiO_(3) and surface passivated Li_(3)PO_(4) layer is deposited on LNMO via a one-step calcination process.As evidenced by transmission electron microscopy(TEM),time-of-flight secondary ion mass spectrometry(ToF-SIMS)and density functional theory(DFT)calculation,the epitaxial growth of LaNiO_(3) along the LNMO lattice can effectively stabilize the structure and inhibit irreversible phase transitions,and the Li_(3)PO_(4) surface coating can prevent the chemical reaction between HF and transition metals without sacrificing the electrochemical activity.In addition,the ionic conductive Li_(3)PO_(4) and atomic wetting inter-layer enables fast charge transfer transport property.Consequently,the LNMO material enabled by the lattice bonding and surface passivating features,demonstrates high performance at high current densities and good capacity retention during long-term test.The rational design of interface coherent engineering and surface coating layers of the LNMO cathode material offers a new perspective for the practical application of high-voltage lithium-ion batteries.

Monothetic and conductive network and mechanical stress releasing layer on micron-silicon anode enabling high-energy solid-state battery

Silicon has ultrahigh capacity,dendrite-free alloy lithiation mechanism and low cost and has been regarded as a promising anode candidate for solid-state battery.Owing to the low infiltration of solid-state electrolyte(SSE),not the unstable solid-electrolyte interphase(SEI),but the huge stress during lithiation-and delithiation-induced particle fracture and conductivity lost tend to be the main issues.In this study,starting with micron-Si,a novel monothetic carbon conductive framework and a MgO coating layer are designed,which serve as electron pathway across the whole electrode and stress releasing layer,respectively.In addition,the in situ reaction between Si and SSE helps to form a LiF-rich and mechanically stable SEI layer.As a result,the mechanical stability and charge transfer kinetics of the uniquely designed Si anode are significantly improved.Consequently,high initial Coulombic efficiency,high capacity and durable cycling stability can be achieved by applying the Si@MgO@C anode in SSB.For example,high specific capacity of 3224.6 mAh·g^(-1)and long cycling durability of 200 cycles are achieved.This work provides a new concept for designing alloy-type anode that combines surface coating on particle and electrode structure design.