Li Dendrite Growth Research Articles

Rare Earth Single-Atom Catalysis for High-Performance Li-S Full Battery with Ultrahigh Capacity.

Lithium-sulfur (Li-S) batteries have many advantages but still face problems such as retarded polysulfides redox kinetics and Li dendrite growth. Most reported single atom catalysts (SACs) for Li-S batteries are based on d-band transition metals whose d orbital constitutes active valence band, which is inclined to occur catalyst passivation. SACs based on 4f inner valence orbital of rare earth metals are challenging for their great difficulty to be activated. In this work, we design and synthesize the first rare earth metal Sm SACs which has electron-rich 4f inner orbital to promote catalytic conversion of polysulfides and uniform deposition of Li. Sm SACs enhance the catalysis by the activated 4f orbital through an f-d-p orbital hybridization. Using Sm-N3C3 modified separators, the half cells deliver a high capacity over 600 mAh g-1 and a retention rate of 84.3 % after 2000 cycles. The fabricated Sm-N3C3-Li|Sm-N3C3@PP|S/CNTs full batteries can provide an ultra-stable cycling performance of a retention rate of 80.6 % at 0.2 C after 100 cycles, one of the best full Li-S batteries. This work provides a new perspective for the development of rare earth metal single atom catalysis in electrochemical reactions of Li-S batteries and other electrochemical systems for next-generation energy storage.

Rare Earth Single‐Atom Catalysis for High‐Performance Li−S Full Battery with Ultrahigh Capacity

AbstractLithium‐sulfur (Li−S) batteries have many advantages but still face problems such as retarded polysulfides redox kinetics and Li dendrite growth. Most reported single atom catalysts (SACs) for Li−S batteries are based on d‐band transition metals whose d orbital constitutes active valence band, which is inclined to occur catalyst passivation. SACs based on 4f inner valence orbital of rare earth metals are challenging for their great difficulty to be activated. In this work, we design and synthesize the first rare earth metal Sm SACs which has electron‐rich 4f inner orbital to promote catalytic conversion of polysulfides and uniform deposition of Li. Sm SACs enhance the catalysis by the activated 4f orbital through an f‐d‐p orbital hybridization. Using Sm‐N3C3 modified separators, the half cells deliver a high capacity over 600 mAh g−1 and a retention rate of 84.3 % after 2000 cycles. The fabricated Sm‐N3C3‐Li|Sm‐N3C3@PP|S/CNTs full batteries can provide an ultra‐stable cycling performance of a retention rate of 80.6 % at 0.2 C after 100 cycles, one of the best full Li−S batteries. This work provides a new perspective for the development of rare earth metal single atom catalysis in electrochemical reactions of Li−S batteries and other electrochemical systems for next‐generation energy storage.

Rational design of polymer-based insulating scaffolds for high-capacity lithium metal batteries

Lithium metal is a promising anode material for next-generation high-energy–density secondary batteries. However, the uncontrolled growth of Li dendrites leads to infinite volume expansion and poor cycling stability. Herein, we propose a designable insulating polydopamine (PDA)-coated porous polytetrafluoroethylene (PTFE) scaffold. A porous PTFE (pPTFE) scaffold with micron-sized pores was fabricated, which provided bottom-up Li deposition owing to its insulating nature. Furthermore, the PDA-coated porous PTFE (PDA-pPTFE) scaffold provided internal space for Li growth and homogenized the Li-ion flux with abundant polar functional groups in the PDA, enabling “bottom-up” Li deposition within the scaffold without dendrite growth. This uniquely designed scaffold demonstrated excellent performance in half and symmetric cells with a small voltage hysteresis and dendrite-free Li plating. Moreover, when coupled with high-loading NCM cathodes (∼4 mA h cm−2), the PDA-pPTFE-based full cells exhibited stable cycling and rate performance, even with a low NP ratio of 1.0 at a rate of 1/3C, and exhibited a high energy density of 801 W h L−1. These results indicated the potential of the PDA-pPTFE scaffold as an anode material for highly stable next-generation rechargeable batteries.

In situ constructing fluorine/nitrogen-enriched interface on highly lithiophilic carbon fiber/MXene/ZnS skeleton for stable lithium anodes

Metallic lithium (Li) is an excellent electrode material for high-energy-density batteries; however, the continuous growth of Li dendrites and the poor deposited volume consistency of Li severely influence the stability of Li anodes. Herein, a LiF-Li3N/LiNxOy-enriched SEI is prepared in situ using a strongly lithiophilic 3D carbon fiber/MXene/ZnS (CMZ) skeleton. Multiscale in situ and ex situ characterizations reveal the mechanisms for Li nucleation and growth on the CMZ skeleton, proving that Li grows tightly over CMZ fibers. This behaviour is attributed to the CMZ skeleton, which provides abundant atomic-level active sites for the uniform and dense nucleation of Li. Electrochemical tests confirm that SEI enriched with LiF-Li3N/LiNxOy can effectively improve Li deposition kinetics, ensure uniform mass transfer and rapid migration of lithium ions in the SEI, and guarantee uniform growth of Li. Consequently, a half cell with a Li-CMZ electrode delivers a high Coulombic efficiency (99.83 %), an ultralong cycling life (17,860 h), and an excellent rate performance (30 mA cm−2). Moreover, full cells consisting of a Li-CMZ anode and different cathodes exhibit superior cycling stabilities. For Li-CMZ ‖ LiFePO4 pouch cell, 84 % capacity is maintained after 300 cycles at 1 C.

Revisiting porous foam Cu host based Li metal anode: The roles of lithiophilicity and hierarchical structure of three-dimensional framework

Lithium (Li) metal anode (LMA) is one of the most promising anodes for high energy density batteries. However, its practical application is impeded by notorious dendrite growth and huge volume expansion. Although the three-dimensional (3D) host can enhance the cycling stability of LMA, further improvements are still necessary to address the key factors limiting Li plating/stripping behavior. Herein, porous copper (Cu) foam (CF) is thermally infiltrated with molten Li-rich Li-zinc (Li-Zn) binary alloy (CFLZ) with variable Li/Zn atomic ratio. In this process, the LiZn intermetallic compound phase self-assembles into a network of mixed electron/ion conductors that are distributed within the metallic Li phase matrix and this network acts as a sublevel skeleton architecture in the pores of CF, providing a more efficient and structured framework for the material. The as-prepared CFLZ composite anodes are systematically investigated to emphasize the roles of the tunable lithiophilicity and hierarchical structure of the frameworks. Meanwhile, a thin layer of Cu-Zn alloy with strong lithiophilicity covers the CF scaffold itself. The CFLZ with high Zn content facilitates uniform Li nucleation and deposition, thereby effectively suppressing Li dendrite growth and volume fluctuation. Consequently, the hierarchical and lithiophilic framework shows low Li nucleation overpotential and highly stable Coulombic efficiency (CE) for 200 cycles in conventional carbonate based electrolyte. The full cell coupled with LiFePO4 (LFP) cathode demonstrates high cycle stability and rate performance. This work provides valuable insights into the design of advanced dendrite-free 3D LMA toward practical application.

Boosted Li+ transport ensured by high-entropy Prussian blue analogues with tuned PF6− adsorption for stable Li metal anode

The inhomogeneous lithium metal (Li) deposition and low lithium ion (Li+) mobility lead to the formation and growth of Li dendrites, which impede the desirable performance of Li metal batteries (LMBs) with high energy density in widely practical applications. Herein, a high-entropy MnCoNiCuZn-Prussian blue analogue (HE-PBA) is utilized to modify the commercial polypropylene separator (PP@HE-PBA), which will form an artificial protective layer on the surface of Li. The polar –CN groups of HE-PBA can enhance the wettability of PP to the electrolyte, while the movement of PF6− anions are flexibly tuned by the appropriate absorption ability and synergistic effect of multiple metal ions in HE-PBA. A high Li+ transference number of 0.69 is achieved, which can relieve the Li+ concentration polarization, regulate the Li+ flow, and realize the uniform Li deposition. With PP@HE-PBA, the Li||Li symmetric cells display durability up to 600 h in the ester-based electrolyte at 1 mA cm−2 for 1 mAh cm−2. Also, the PP@HE-PBA exhibits great potential in LMBs, where the Li4Ti5O12 (LTO) ||Li and sulfated polyacrylonitrile (S-PAN) ||Li batteries deliver superior cycling performance to those without PP@HE-PBA.

In Situ Interphasial Engineering Enabling High‐Rate and Long‐Cycling Li Metal Batteries

AbstractThe practical implementation of Li metal anode has long been hindered by the significant challenges of notorious dendritic Li growth and severe interphase instability during repeated cycling. Herein, a highly lithiophilic NiSe‐modified host has rationally been constructed to stabilize Li metal by the facile mechanical rolling strategy. The in situ configurated high‐flux Li2Se‐enriched interphase layer can facilitate the fast interfacial charge transfer, high Li plating/stripping reversibility and homogeneous Li nucleation/growth. Consequently, the achieved modified Li metal demonstrates ultrahigh rate capability (10 mA cm−2) and ultralong‐term cycling stability (6600 cycles) with dendrite‐free Li deposition. The Li|LiFePO4 (LFP) cell exhibits an extraordinarily long lifespan cycling stability over 500 cycles with an ultra‐low decay rate of only ≈0.0092% per cycle at 1 C. Furthermore, the 4.5 V high‐voltage Li|LiCoO2 pouch cell with a high areal capacity (≈1.9 mAh cm−2) still reveals an impressively prolonged cyclability over 200 cycles even under the harsh test condition of low negative‐to‐positive‐capacity (N/P) ratio of ≈3.4 and lean electrolyte of ≈5.5 µL mAh−1. This work provides a facile and scalable strategy toward a highly stable Li metal anode for reliable practical usage.

A novel polymeric lithicone coating for superior lithium metal anodes

Lithium metal (Li) is commonly regarded as the “holy grail” of rechargeable batteries and can serve as anodes for constituting various high-energy lithium metal batteries (LMBs). However, it suffers from two notorious issues: (1) continuous formation of inhomogeneous solid electrolyte interphase and (2) Li dendritic growth. In this study, we developed a novel polymeric lithicone via a new molecular layer deposition (MLD) process, using lithium tert-butoxide (LTB) and hydroquinone (HQ) as precursors. We revealed that such an MLD process enabled the resultant LiHQ to grow linearly in a highly controllable and cyclic mode at a growth rate of 4 Å cycle−1. Furthermore, its low process deposition temperature of 150 °C made it possible to practice high-quality coatings over Li anodes directly. We demonstrated that, very compellingly, this LiHQ coating could protect Li anodes from corrosion and dendritic growth. As a consequence, this LiHQ coating has enabled Li||Li symmetric cells an extremely long cyclability up to 8000 Li-plating/stripping cycles without failure. More excitingly, we demonstrated that, coupled with LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes, the LiHQ-modified Li anodes could help the resultant Li||NMC811 realize a much better capacity retention and much longer cyclability. Thus, this study represents a strategic route for developing commercializeable LMBs.

Imidazolium bromide based dual-functional redox mediator for the construction of dendrite-free Li-CO2 batteries

Rechargeable lithium-carbon dioxide (Li-CO2) batteries have emerged as a highly promising approach to simultaneously address energy shortages and the greenhouse effect. However, certain limitations exist in Li-CO2 batteries like high charge overpotential and unstable Li metal interface, which adversely affect the energy efficiency and cycling life. The incorporation of soluble redox mediators (RMs) has proven effective in enhancing the charge transfer between lithium carbonate (Li2CO3) and cathode, thereby substantially reducing the charge overpotential. Nevertheless, the severe shuttle effect of RMs results in the reactions with Li anode, not only exacerbating the corrosion of Li anode but also leading to the depletion of RMs and electrical energy efficiency. In this work, an organic compound containing large cation group, 1-ethyl-3-methylimidazole bromide (EMIBr) is proposed as the defense donor RM for Li anode in Li-CO2 batteries to address the above problems simultaneously. During charging, Li2CO3 oxidation kinetics can be accelerated by bromide anion pair (Br3−/Br−). Meanwhile, the cations (EMI+) are preferentially adsorbed around the protruding tips of Li anode through electrostatic interaction driven by surface free energy, forming protective layers that effectively inhibit further Li deposition at these tips, which is verified by DFT calculations. Additionally, Li dendrites growth is inhibited by the electrostatic repulsion of polar groups in EMIBr, resulting in uniform Li deposition. Consequently, a lower overpotential (∼1.17 V) and a longer cycle life (∼200 cycles) have been obtained for Li-CO2 battery incorporating EMIBr.

Interfacial modulation of bifunctional electrolyte additive engineering for dendrite-free and robust lithium metal anode

Anode materials for rechargeable electric car batteries are obtained from Li-metal owing to their extremely high specific capacity and low redox potential. Unfortunately, safety concerns related to dendrite formation on the anode surface caused by the uneven distribution of Li-ions during the discharge process interfere with the use of Li-metal in industrial batteries. In this study, methyl vinyl sulfone (MVS), a sulfone-based functional electrolyte additive, is used in an additive engineering strategy to control Li-electrolyte interactions and address the aforementioned problems. Li dendrite growth may be restricted, and transition metal degradation on the surface of the cathode can be reduced by the MVS-derived functional electrolyte additive interfacial layer. The electrochemical performance of an ethylene carbonate/dimethyl carbonate (EC/DMC) + 1 wt% MVS Li-metal anode of a Li||Li symmetric cell exhibits remarkable cycle stability, maintaining a low overvoltage for over 750 h at 1 mA cm−2, and capacity of 1 mA h cm−2. Additionally, LiNi0.8Co0.1Mn0.1O2 (NCM811) full cells with the MVS additive exhibit enhanced electrochemical stability for 250 cycles at a current density of 100 mA g−1. This study provides an innovative approach for stabilizing the metal-electrolyte interfacial layer that may be used for practical applications in metal-based rechargeable batteries.

Ingenious separator architecture: Revealing the versatile 3D heterostructured MXene-hydrogen titanate electrocatalysts for advanced lithium-sulfur battery

Lithium-sulfur batteries (LSBs) with high theoretical energy density and cost-effectiveness have great promise as alternative energy storage systems to traditional lithium-ion batteries. Nevertheless, their practical application is severely hindered due to a myriad of shortcomings such as “shuttling effect” of lithium polysulfides (LiPSs), sluggish conversion kinetics of sulfur (S) species, low electrical conductivity of S and discharged products, and intractable lithium dendrite growth. Herein, a novel 3D-heterostructured electrocatalyst consisting of the in-situ grown H2Ti3O7 (HTO) nano-whiskers on a Ti3C2Tx (MXene) substrate (M-HTO-0.5) is designed using a MXene-derived hydrothermal process combined with following ion exchange between Na+ and H+, wherein the hydrothermal reaction time regulation (0.5 h) mainly induces the balanced co-existence of HTO and MXene in the microstructure of M-HTO-0.5. Benefiting from the synergistic effect between M-HTO-0.5 (strong LiPS chemisorption, outstanding catalytic activity with abundant active sites, and boosted Li+ ion migration) and carbon nanotubes (CNTs) (construction of ion/electron transport network), the ingenious design of multi-functional separators (M-HTO-0.5-C) effectively restricts LiPS shuttling and dendritic Li growth simultaneously. Consequently, LSBs with M-HTO-0.5-C separators achieve remarkable rate capability, and stable long-term cyclability even at 5.0 C. This study opens an innovative avenue for developing high-performance LSB configurations.

Coupling of ion-conducting interphase with lithiophilic-solid-oxide-electrolyte interlayer toward fast-charging lithium metal batteries

The uncontrollable dendritic Li growth and limited Coulombic efficiency have long impeded the implementation of fast-charging lithium metal batteries. Contrary to the widely accepted attempt of using a sintering dense ceramic electrolyte to realize dendrite-free deposition, we report a coupling architecture of ion-conducting-Li3PO4-Li3N interphase with lithiophilic-solid-oxide-electrolyte interlayer for Li-metal anode using a reactive lithiophilic solid oxide electrolyte (RLSE) rather than dense ceramics. The synergistic interphase and protection layer can facilitate the Li-ion transport and enhance the lithiophilicity. As a result, an ultrahigh Li plating/stripping current density of 10 mA cm−2 and areal capacity of 10 mAh cm−2 for over 1000 h, and a remarkable Coulombic efficiency of 99.8 % are achieved simultaneously. Moreover, the use of interphase-interlayer synergistic protection enables a stable long-term 3000-cycling of Li||Li4Ti5O12 cell at 2C rate. More importantly, high-current–density (e.g. 1.8 mA cm−2) cycling of Li||LiNi0.8Co0.1Mn0.1O2 batteries with a practical area capacity of 3.6 mAh cm−2 is achieved in both carbonate and quasi-solid electrolytes. This study demonstrates an alternative approach of solid oxide electrolytes to stabilize Li-metal anode and enable fast-charging lithium metal batteries.

Li (200) with in-situ generated high entropy alloy/oxide fillers and Li2O enabling desirable Li metal anode

The development of Li metal batteries (LMBs) with high-energy density is impeded by the uncontrollable growth of Li dendrites. In this work, the Li foil is cold-pressed with ball-milled high entropy Mg/Ni/Co/Cu/Zn-based oxides (HEO), which can in-situ generate high entropy alloy/oxide and Li2O in the bulk phase and surface of composited Li anode (denoted as HEA/O@Li). During the cold-pressing process, the Li foil with polycrystalline nature transform into (200) textured Li. The in-situ generated Li2O can provide more lithiophilic sites and enrich the inorganic components of solid state interface (SEI), while the HEA/O fillers dispersed in the composited Li anode can strength corresponding mechanical stability and tune the Li+ stripping/plating process. As a result, the HEA/O@Li exhibits outstanding cycle stability for almost 1000 h at 1 mA cm−2 with fixed area capacity of 1 mAh cm−2. Moreover, the full batteries matched with LiFePO4 cathode demonstrate favorable cycling stability (110 mAh g−1 at 0.5C after 700 cycles) and rate capability.

Multiple uniform lithium-ion transport channels in Li6.4La3Zr1.4Ta0.6O12/Ce(OH)3 modified polypropylene composite separator for high-performance lithium metal batteries

Lithium (Li) metal anodes (LMAs) are regarded as leading technology for advanced-generation batteries due to their high theoretical capacity and favorable redox potential. However, the practical integration of LMAs into high-energy rechargeable batteries is hindered by the challenge of Li dendrite growth. In this work, nanoparticles of Li6.4La3Zr1.4Ta0.6O12 (LLZTO) loaded with Ce(OH)3 (LLZTCO) were designed and synthesized by a hydrothermal method. A functional composite separator was crafted by coating one side of a polypropylene (PP) separator with a composite electrolyte comprised of polyvinylidene fluoride (PVDF) and LLZTCO. The synergistic interactions between PVDF and LLZTCO provide numerous rapid lithium-ion (Li+) channels, facilitating the efficient redistribution of disparate Li+ flux originating from the insulated PP separator. The composite separator demonstrated an ionic conductivity (σ) of 3.68 × 10–3 S cm−1, substantial Li+ transference number (t+) of 0.73, and a high electrochemical window of 4.8 V at 25℃. Furthermore, the Li/LLZTCO@PP/Li symmetric cells demonstrated stable cycling for over 2000 h without significant dendrite formation. The Li/LiFePO4 (LFP) cells assembled with LLZTCO@PP separators exhibited a capacity retention of 91.6 % after 400 cycles at 1C. This study offers a practical approach to fabricating composite separators with enhanced safety and superior electrochemical performance.

Enhancing Lithium-Ion Diffusion Kinetics in a 3D Lithium Metal Host through Surface Modification with Hierarchical Multimetal Oxides.

Lithium metal is a promising anode candidate to achieve high-energy-density lithium metal batteries (LMBs) due to its ultrahigh theoretical capacity (3860 mA h g-1) and low electrochemical potential (-3.04 V vs S.H.E). Unfortunately, the commercialization of lithium metal anodes is hindered by the growth of Li dendrites and the infinite Li volume changes during the cycling process. Herein, we introduce a 3D hierarchical multimetal oxide nanowire framework as a current collector for Li metal anodes. The hierarchical metal oxide layers of CoO and CuxO provide abundant Li nucleation sites and thus offer uniform Li plating and regulate Li nucleation during the charge/discharge process. As a result, half cells present a prolonging Coulombic efficiency of 97% at 1 mA cm-2 with a capacity of 1 mA h cm-2 for over 300 cycles. A stable cyclability of symmetric cells is demonstrated under 1 mA cm-2 with a capacity of 1 mA h cm-2 for 1500 h. Full cells paired with an LFP cathode show a stable capacity of 131.5 mA h g-1 with a capacity retention of 92% for 200 cycles. These results will shed insights into the design of 3D Cu current collectors for high-performance composite Li metal anodes.

Realizing Ultrathin LiSn Alloy Anode by Tuning the Wettability of Molten Li for High-Energy-Density Batteries.

Despite being heralded as the "holy grail" of anodes for their high theoretical specific capacity, lithium (Li) metal anodes still face practical challenges due to difficulties in fabricating ultrathin Li with controllable thickness and suppressing Li dendrites growth. Herein, we introduce a simple and cost-effective dip-coating method to fabricate ultrathin lithium-tin (LiSn) anode with adjustable thicknesses ranging from 4.5 to 45 μm. The in situ formation of Li22Sn5 alloy improves the wettability of the molten Li, enabling the casting of ultrathin Li metal layers on different substrates. More importantly, the abundant Li22Sn5 lithiophilic sites significantly lower the nucleation overpotential, inducing uniform Li deposition and accelerating the electrochemical reaction at the interface. As a result, the symmetric cell assembled with LiSn-Cu electrodes can cycle stably for more than 120 h with a charge/discharge depth of 50%, which is 1.5 times longer than the lifespan of the pure Li anode. In the full cells paired with NCM cathode, the discharge specific capacity is improved from 13.84 to 70.31 mA h g-1 with the LiSn-Cu anode at 8 C. The LiSn-Cu||NCM full cell realized a high energy density of 724.9 Wh kg-1 at the active material level with an N/P ratio of 1.4.

Double-Salts Super Concentrated Carbonate Electrolyte Boosting Electrochemical Performance of Ni-Rich LiNi0.90Co0.05Mn0.05O2 Lithium Metal Batteries.

Current lithium-ion batteries cannot meet the requirement of higher energy density with further large-scale application of electrical vehicles. Lithium metal batteries combined with Ni-rich layered oxides cathode are expected as the one of promising solutions, while the poor electrode and electrolyte interface impedes the commercial development of lithium metal batteries. A new double-salts super concentrated (DSSC) carbonate electrolyte is proposed to improve the electrochemical performance of LiNi0.90Co0.05Mn0.05O2 (NCM9055)||Li metal battery which exhibits stable cycling performance with the capacity retention of 93.04% and reversible capacity of 173.8 mAh g-1 after 100 cycles at 1 C, while cells with conventional 1m diluted electrolyte remains only 60.55% and capacity of 114.2 mAh g-1. The double salts synergistic effect in super concentrated electrolyte promotes the formation for more balanced stable cathode electrolyte interface (CEI) inorganic compounds of CFx, LiNOx, SOF2, Li2SO4, and less LiF by X-ray photoelectron spectroscopy (XPS)test, and the uniform 2-3nm rock-salt phase protection layer on the cathode surface by transmission electron microscope (TEM) characterization, improving the cycling performance of the Ni-rich NCM9055 layered oxide cathode. The DSSC electrolyte also can relief the Li dendrite growth on Li metal anode, as well as exhibit better flame retardance, promoting the application of more safety Ni-rich NCM9055||Li metal batteries.

Design of Fluorinated Elastomeric Electrolyte for Solid-State Lithium Metal Batteries Operating at Low Temperature and High Voltage.

This work demonstrates the low-temperature operation of solid-state lithium metal batteries (LMBs) through the development of a fluorinated and plastic-crystal-embedded elastomeric electrolyte (F-PCEE). The F-PCEE is formed via polymerization-induced phase separation between the polymer matrix and plastic crystal phase, offering a high mechanical strain (≈300%) and ionic conductivity (≈0.23 mS cm-1) at -10°C. Notably, strong phase separation between two phases leads to the selective distribution of lithium (Li) salts within the plastic crystal phase, enabling superior elasticity and high ionic conductivity at low temperatures. The F-PCEE in a Li/LiNi0.8Co0.1Mn0.1O2 full cell maintains 74.4% and 42.5% of discharge capacity at -10°C and -20°C, respectively, compared to that at 25°C. Furthermore, the full cell exhibits 85.3% capacity retention after 150 cycles at -10°C and a high cut-off voltage of 4.5V, representing one of the highest cycling performances among the reported solid polymer electrolytes for low-temperature LMBs. This work attributes the prolonged cycling lifetime of F-PCEE at -10°C to the great mechanical robustness to suppress the Li-dendrite growth and ability to form superior LiF-rich interphases. This study establishes the design strategies of elastomeric electrolytes for developing solid-state LMBs operating at low temperatures and high voltages.

Stable Lithium Metal Batteries Enabled by Lithiophilic Core-Shell Nanowires on Copper Foam.

Lithium (Li) metal batteries have attracted considerable research attention due to their exceptionally high theoretical capacity. However, the commercialization of Li metal batteries faces challenges, primarily attributed to uncontrolled growth of Li dendrites, which raises safety concerns and lowers coulombic efficiency. To mitigate Li dendrites growth and attain dense Li deposition, the hybrid SiO2-Cu2O lithiophilic film applied to a 3D copper foam current collector is developed to regulate the interfacial properties for achieving even and dense Li deposition. The SiO2-Cu2O possesses strong Li+ trapping capability through strong lithiophilicity from Cu2O. Additionally, the SiO2-Cu2O enables uniform ion diffusion through the domain-limiting effect of the holes in the SiO2 layer, inducing an even and dense Li plating/stripping behavior at a large capacity. Furthermore, the SiO2 layer promotes the formation of an initial high inorganic content Solid Electrolyte Interphase (SEI) through selective preferential binding with anion and solvent molecules. When the SiO2-Cu2O@Li anode is coupled with a LiFePO4 (LFP) cathode, the resulting full cell exhibits superior cycling stability and rate performance. These results provide a facile approach to construct a lithiophilic current collector for practical Li metal anodes.

Scalable Customization of Crystallographic Plane Controllable Lithium Metal Anodes for Ultralong-Lasting Lithium Metal Batteries.

A formidable challenge to achieve the practical applications of rechargeable lithium (Li) metal batteries (RLMBs) is to suppress the uncontrollable growth of Li dendrites. One of the most effective solutions is to fabricate Li metal anodes with specific crystal plane, but still lack of a simple and high-efficient approach. Herein, a facile and controllable way for the scalable customization of polished Li metal anodes with highly preferred (110) and (200) crystallographic orientation (donating as polished Li(110) and polished Li(200), respectively) by regulating the times of accumulative roll bonding, is reported. According to the inherent characteristics of polished Li(110)/Li(200), the influence of Li atomic structure on the electrochemical performance of RLMBs is deeply elucidated by combining theoretical calculations with relative experimental proofs. In particular, a polished Li(110) crystal plane is demonstrated to induce Li+ uniform deposition, promoting the formation of flat and dense Li deposits. Impressively, the polished Li(110)||LiFePO4 full cells exhibit unprecedented cycling stability with 10000 cycles at 10 C almost without capacity degradation, indicating the great potential application prospect of such textured Li metal. More valuably, this work provides an important reference for low-cost, continued, and large-scale production of Li metal anodes with highly preferred crystal orientation through roll-to-roll manufacturability.