Suppressing dendritic metallic Li formation on graphite anode under battery fast charging

Lithium-ion batteries(LIBs)with fast-charging capability are essential for enhancing consumer experience and accelerating the global market adoption of electric vehicles.However,achieving fast-charging capability without compromising energy density,cycling lifespan,and safety of LIBs remains a significant challenge due to the formation of dendritic Li metal on graphite anode under fast charging condition.In view of this,the fundamentals for the dendritic metallic Li formation and the strategies for suppressing metallic Li plating based on analyzing the entire Li^(+)transport pathway at the anode including electrolyte,pore structure of electrode,and surface and bulk of materials are summarized and discussed in this review.Besides,we highlight the importance of designing thick electrodes with fast Li^(+)transport kinetics and comprehensively understanding the interaction between solid electrolyte interphase(SEI)and Li^(+)migration in order to avoid the formation of dendritic Li metal in practical fast-charging batteries.Finally,the regulation of Li metal plating with plane morphology,instead of dendritic structure,on the surface of graphite electrode under fast-charging condition is analyzed as a future direction to achieve higher energy density of batteries without safety concerns.

Stress-Regulation Design of Lithium Alloy Electrode toward Stable Battery Cycling

Metallic tin(Sn)foil is a promising candidate anode for lithium-ion batteries(LIBs)due to its metallurgical processability and high capacity.However,it suffers low initial Coulombic efficiency and inferior cycling stability due to its uneven alloying/dealloying reactions,large volume change and stress,and fast electrode structural degradation.Herein,we report an undulating LiSn electrode fabricated by a scalable two-step procedure involving mechanical lithography and chemical prelithiation of Sn foil.With the combination of experimental measurements and chemo-mechanical simulations,it was revealed the obtained undulating LiSn/Sn electrode could ensure better mechanical stability due to the pre-swelling state from Sn to Li x Sn and undulating structure of lithography in comparison with plane Sn,homogenize the electrochemical alloying/dealloying reactions due to the activated surface materials,and compensate Li loss during cycling due to the introduction of excess Li from Li_(x)Sn,thus enabling enhanced electrochemical performance.Symmetric cells consisting of undulating LiSn/Sn electrode with an active thickness of∼5 um displayed stable cycling over 1000 h at 1 mA cm^(-2) and 1 mAh cm^(-2) with a low average overpotential of<15 mV.When paired with commercial LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)cathode with high mass loading of 15.8 mg cm^(-2),the full cell demonstrated a high capacity of 2.4 mAh cm^(-2) and outstanding cycling stability with 84.9% capacity retention at 0.5 C after 100 cycles.This work presents an advanced LiSn electrode with stress-regulation design toward high-performance LIBs,and sheds light on the rational electrode design and processing of other high-capacity lithium alloy anodes.

Insights on“nitrate salt”in lithium anode for stabilized solid electrolyte interphase

A Li/KNO_(3) composite(LKNO),with KNO_(3) uniformly implanted in bulk metallic Li,is fabricated for battery anode via a facile mechanical kneading approach,which exhibits high Coulombic efficiency and prolonged cycle life.The mechanism behind the enhanced electrochemical performance of the“salt-in-metal”composite is investigated,where KNO_(3) in metallic Li composite electrode would be sustainably released into the electrolyte.The presence of NO_(3)-stabilizes the solid electrolyte interphase by producing functional Li_(3)N,LiNxOy,and Li_(2)O species.K^(+)from KNO_(3) also helps to form an electrostatic shield after its adsorption on the electrode protrusions,which suppresses the dendritic growth of metallic Li.With the above advantages,uniform Li plating with dense and planar structure is realized for the LKNO electrode.These findings reveal a deep understanding of the effect of the“saltin-metal”anode and provide new insights into the use of nitrate additives for high-energy-density Li metal batteries.

A Li_(3)P nanoparticle dispersion strengthened ultrathin Li metal electrode for high energy density rechargeable batteries

Achievement of lithium(Li)metal anode with thin thickness(e.g.,≤30µm)is highly desirable for rechargeable high energy density batteries.However,the fabrication and application of such thin Li metal foil electrode remain challenging due to the poor mechanical processibility and inferior electrochemical performance of metallic Li.Here,mechanico-chemical synthesis of robust ultrathin Li/Li_(3)P(LLP)composite foils(~15µm)is demonstrated by employing repeated mechanical rolling/stacking operations using red P and metallic Li as raw materials.The in-situ formed Li+-conductive Li_(3)P nanoparticles in metallic Li matrix and their tight bonding strengthen the mechanical durability and enable the successful fabrication of free-standing ultrathin Li metal composite foil.Besides,it also reduces the electrochemical Li nucleation barrier and homogenizes Li plating/stripping behavior.When matching to high-voltage LiCoO_(2),the full cell with a low negative/positive(N/P)capacity ratio of~1.5 offers a high energy density of~522 W·h·kg^(-1) at 0.5 C based on the mass of cathode and anode.Taking into account its facile manufacturing,potentially low cost,and good electrochemical performance,we believe that such an ultrathin composite Li metal foil design with nanoparticle-dispersion-strengthened mechanism may boost the development of high energy density Li metal batteries.

General deep learning framework for emissivity engineering

Wavelength-selective thermal emitters(WS-TEs)have been frequently designed to achieve desired target emissivity spectra,as a typical emissivity engineering,for broad applications such as thermal camouflage,radiative cooling,and gas sensing,etc.However,previous designs require prior knowledge of materials or structures for different applications and the designed WS-TEs usually vary from applications to applications in terms of materials and structures,thus lacking of a general design framework for emissivity engineering across different applications.Moreover,previous designs fail to tackle the simultaneous design of both materials and structures,as they either fix materials to design structures or fix structures to select suitable materials.Herein,we employ the deep Q-learning network algorithm,a reinforcement learning method based on deep learning framework,to design multilayer WS-TEs.To demonstrate the general validity,three WS-TEs are designed for various applications,including thermal camouflage,radiative cooling and gas sensing,which are then fabricated and measured.The merits of the deep Q-learning algorithm include that it can(1)offer a general design framework for WS-TEs beyond one-dimensional multilayer structures;(2)autonomously select suitable materials from a self-built material library and(3)autonomously optimize structural parameters for the target emissivity spectra.The present framework is demonstrated to be feasible and efficient in designing WS-TEs across different applications,and the design parameters are highly scalable in materials,structures,dimensions,and the target functions,offering a general framework for emissivity engineering and paving the way for efficient design of nonlinear optimization problems beyond thermal metamaterials.