Revealing the importance of suppressing formation of lithium hydride and hydrogen in Li anode protection

The reviving of the“Holy Grail”lithium metal batteries(LMBs)is greatly hindered by severe parasitic reactions between Li anode and electrolytes.Herein,first,we comprehensively summarize the failure mechanisms and protection principles of the Li anode.Wherein,despite being in dispute,the formation of lithium hydride(LiH)is demonstrated to be one of the most critical factors for Li anode pulverization.Secondly,we trace the research history of LiH at electrodes of lithium batteries.In LMBs,LiH formation is suggested to be greatly associated with the generation of H_(2)from Li/electrolyte intrinsic parasitic reactions,and these intrinsic reactions are still not fully understood.Finally,density functional theory calculations reveal that H_(2)adsorption ability of representative Li anode protective species(such as LiF,Li_(3)N,BN,Li_(2)O,and graphene)is much higher than that of Li and LiH.Therefore,as an important supplement of well-known lithiophilicity theory/high interfacial energy theory and three key principles(mechanical stability,uniform ion transport,and chemical passivation),we propose that constructing an artificial solid electrolyte interphase layer enriched of components with much higher H_(2)adsorption ability than Li will serve as an effective principle for Li anode protection.In summary,suppressing formation of LiH and H_(2)will be very important for cycle life enhancement of practical LMBs.

Unshackling the reversible capacity of SiO_(x)/graphite-based full cells via selective LiF-induced lithiation

Composite Si@SiO_(x)/C anodes with high specific capacity are considered the most promising alternatives to graphite in industrial lithium-ion batteries.However,their cycling stability remains a limiting factor,which originates from the severe volume deformation of silicon-derived species.In this work,the cyclabilities of composite anodes are improved by unshackling the highly reversible lithium storage capabilities from the redundancy capacity of the anode materials.A selective LiF-induced lithiation strategy is proposed based on exploiting interface separation energy differences between LiF and the active materials.An interesting preferential redeposition of LiF is observed at the Si@SiO_(x) particles,which differentiates the otherwise similar lithiation potentials of LiC_(x) and Li_(15)Si_(4),thereby enabling lithium storage in graphite that was previously underused.The resulting full cell exhibits better rate and cycling performances without sacrificing specific capacity.In an ultra-high area capacity full cell(4.9 mA h cm^(-2)),the capacity retention increases markedly from 66.1% to 94.2% after 300 cycles.The selective lithiation strategy developed herein is feasible for practical industrial applications,and importantly,it requires no changes to the existing mature lithium-ion battery manufacturing process.This study offers a new approach for the development of silicon/graphite composite anodes with long cycling lifetimes.

Cu_2GeS_3 derived ultrafine nanoparticles as high-performance anode for sodium ion battery

Germanium based sulfides are potentially attractive as anode material for sodium ion batteries but rarely investigated. Herein, we firstly investigated Na^＋storage properties of pristine Cu2GeS3（PCGS） and found an effective strategy to improve its performance by a single lithiation/delithiation cycle obtaining ultrafine nanoparticle copper germanium sulfide（NCGS）. The lithiation/delithiation process leads to the formation of a stable Li-containing solid electrolyte interphase film and a significant improvement of sodiation kinetics. Therefore, the NCGS anode delivers favorable capacity retention and better rate capability compared with that of a PCGS whether in the half cell or in the full cell,showing great promise for energy storage application.