Drastic Volume Change Research Articles

Nano‐ZnFe2O4 Facilitates Lithium Metal Anode Achieving High Stability

AbstractDue to its remarkably low redox potential and high specific capacity, the lithium metal anode has long been regarded as the ultimate choice for anode in lithium‐ion cells. However, its practical application has been impeded by two major challenges: poor Coulomb efficiency and the inevitable formation of lithium dendrites during charging/discharging processes. In this study, we propose a method to address these issues by fabricating a protective layer for the lithium metal anode using a polyethylene separator that has been modified with a composite of zinc nanoferrite and porous carbon (referred to as ZnFe2O4@PE). By employing this approach, we aim to achieve enhanced stability during anode cycling. The ZnFe2O4@PE serves multiple purposes. Firstly, it effectively reduces the local current density, thereby mitigating the drastic volume changes that occur during charging and discharging. Additionally, the nano‐ZnFe2O4 possesses a favorable affinity for lithium ions, facilitating their homogeneous deposition and suppressing the growth of lithium dendrites. As a result, the lithium metal anodes coated with the ZnFe2O4@PE protective layer exhibit excellent cycling stability, maintaining stable performance for 250 h. This innovative strategy offers a promising application pathway for lithium metal anodes.

A Conductive Binder Based on Mesoscopic Interpenetration with Polysulfides Capturing Skeleton and Redox Intermediates Network for Lithium Sulfur Batteries

AbstractThe practical application of lithium‐sulfur batteries with high theoretical energy density and readily available cathode active materials is hampered by problems such as sulfur insulation, dramatic volume changes, and polysulfide shuttling. The targeted development of novel binders is the most industrialized solution to the problem of sulfur cathodes. Herein, an aqueous conductive emulsion binder with the sulfonate‐containing hard elastic copolymer core and the conjugate polymer shell, which is capable of forming a bicontinuous mesoscopic interpenetrating polymer network, is synthesized and investigated. Not only can the elastic skeleton formed by the copolymer bind the active substance under drastic volume changes, but also the rich ester and cyanide groups in it can effectively capture lithium polysulfide. Meanwhile, the conducting skeleton consisting of poly(3,4‐ethylenedioxythiophene) both provides the additional charge conduction pathways and acts as the redox intermediates, significantly accelerating the kinetic process of lithium polysulfide conversion. Based on the synergistic effect of the above mechanisms, the use of the prepared binder on the sulfur carbon cathode significantly improves the rate performance and cycle stability of lithium sulfur batteries.

A Conductive Binder Based on Mesoscopic Interpenetration with Polysulfides Capturing Skeleton and Redox Intermediates Network for Lithium Sulfur Batteries.

The practical application of lithium-sulfur batteries with high theoretical energy density and readily available cathode active materials is hampered by problems such as sulfur insulation, dramatic volume changes, and polysulfide shuttling. The targeted development of novel binders is the most industrialized solution to the problem of sulfur cathodes. Herein, an aqueous conductive emulsion binder with the sulfonate-containing hard elastic copolymer core and the conjugate polymer shell, which is capable of forming a bicontinuous mesoscopic interpenetrating polymer network, is synthesized and investigated. Not only can the elastic skeleton formed by the copolymer bind the active substance under drastic volume changes, but also the rich ester and cyanide groups in it can effectively capture lithium polysulfide. Meanwhile, the conducting skeleton consisting of poly(3,4-ethylenedioxythiophene) both provides the additional charge conduction pathways and acts as the redox intermediates, significantly accelerating the kinetic process of lithium polysulfide conversion. Based on the synergistic effect of the above mechanisms, the use of the prepared binder on the sulfur carbon cathode significantly improves the rate performance and cycle stability of lithium sulfur batteries.

Preparation and electrochemical properties of flexible self-supported graphene/silicon/carbon nanotube composite electrode for lithium-ion battery

To meet the demand of flexible devices, it was urgent to develop flexible high-capacity electrodes for lithium-ion batteries (LIBs). Silicon (Si) as an active material would effectively elevate the specific capacity of LIBs, but the drastic volume changes and low intrinsic conductivity seriously affected its electrochemical performance during the charge-discharge process. In this research, a new type of composite was designed using two-dimensional reduced graphene oxide (rGO), one-dimensional carbon nanotubes (CNTs), and silicon nanoparticles (Si NPs) as raw materials. The prepared rGO/Si/CNTs composite had an intricate and intersecting porous network structure inside, with rGO as the substrate, CNTs as a bridge, and Si NPs as the active material. The rGO would provide abundant attachment sites for Si NPs, improve electrode conductivity, and alleviate the volume change of electrode. CNTs can effectively suppress the stacking of rGO layers and generate more voids for the reaction, and also serve as a bridge for electron transfer between rGO layers. Furthermore, the interaction between each other also heightened the flexibility and strength of electrodes. Compared to the other composites, rGO/Si/CNTs=2:2:1 electrodes presented the superior electrochemical performance. When cycled at 200 mA g−1, its discharge capacity was 2217.2 mAh g−1 after 200 cycles. As the current density increasing to 1000 and 5000 mA g−1, the discharge capacity maintained at 1877.2 and 534.8 mAh g−1 for 1000th cycle, and it also demonstrated superior rate performance. Besides, the assembled flexible battery maintained a good current output under various bending conditions, and was expected to be widely used in the flexible wearable energy storage devices.

Bionic Capsule Lithium-Ion Battery Anodes for Efficiently Inhibiting Volume Expansion.

Magnetite (Fe3O4) has a large theoretical reversible capacity and rich Earth abundance, making it a promising anode material for LIBs. However, it suffers from drastic volume changes during the lithiation process, which lead to poor cycle stability and low-rate performance. Hence, there is an urgent need for a solution to address the issue of volume expansion. Taking inspiration from how glycophyte cells mitigate excessive water uptake/loss through their cell wall to preserve the structural integrity of cells, we designed Fe3O4@PMMA multi-core capsules by microemulsion polymerization as a kind of anode materials, also proposed a new evaluation method for real-time repair effect of the battery capacity. The Fe3O4@PMMA anode shows a high reversible specific capacity (858.0 mAh g-1 at 0.1 C after 300 cycles) and an excellent cycle stability (450.99 mAh g-1 at 0.5 C after 450 cycles). Furthermore, the LiNi0.8Co0.1Mn0.1O2/Fe3O4@PMMA pouch cells exhibit a stable capacity (200.6 mAh) and high-capacity retention rate (95.5 %) after 450 cycles at 0.5 C. Compared to the original battery, the capacity repair rate of this battery is as high as 93.4 %. This kind of bionic capsules provide an innovative solution for improving the electrochemical performance of Fe3O4 anodes to promote their industrial applications.

Radial channel boosting stress release in hollow carbon spheres for high-rate sodium ions storage

Carbon spheres are appealing anode materials for advanced sodium ions batteries. However, several major hurdles to address are the stress-accumulation associated with the drastic volume change, the sluggish sodium ions diffusion kinetics, and poor electrochemically active sites inside. Herein, the von Mises stress distribution uncovers the critical role of the radial channel on the strain relaxation behavior based on the finite element method. Based on the finite element simulation, the radial porous hollow carbon spheres are proposed and synthesized by a universal strategy with a hard-template approach and dynamic graphitization. RPHCSs dominate opened micro-mesoporous features through the shell. With fast sodium ion diffusivity kinetics and much more accessible electrochemical active sites in shell, RPHCSs electrodes deliver a high specific capacity of 103.0 mAh g−1 even at 4000 mA g−1 with a high capacity contribution ratio > 0.1 V (81.1 %), suggesting its great superiority in the application of high-rate sodium ions storage. Such architecture provides a promising structural platform for the fabrication of high-performance carbon spheres material for other electrochemical energy storage systems.

Constructing Si/6H-SiC Heterostructure As a High-Performance Anode for Boosting Lithium-Ion Storage.

Silicon (Si) anodes offer significant potential due to their high capacity. However, their drastic volume change limits their utility, resulting in a shorter cycling life. In this paper, microsilicon particles and 6H-SiC particles were ball-milled and subsequently coated a layer of amorphous carbon, yielding Si/SiC@C composites. Computational and experimental results reveal that this heterostructure formed between Si and 6H-SiC enhances the electronic conductivity of the Si/SiC@C composites dramatically, as well as the Li ion diffusion rate. Thereby, the Si/6H-SiC heterostructure increases capacity and enhances the rate capability of the Si-based anode. Significantly, the conductivity of Si/SiC@C composites surpasses that of Si@C composites by a factor of around 330. Furthermore, tough, evenly distributed, and electrochemically inert 6H-SiC serves as a rigid framework. By reducing the expansion rate of Si-based anodes and mitigating mechanical stress during cycles, this improves the cycling stability. Additionally, the Si/SiC@C anodes demonstrate superior cycle performance (814.6 mAh g-1 at 1 A g-1 after 400 cycles with capacity retention of 88.0%) and excellent rate capability (762 mAh g-1 at 5 A g-1).

Heterostructure Engineering Enables MoSe2 with Superior Alkali-Ion Storage

Molybdenum diselenide (MoSe2) is a promising anode for alkali-ion storage due to its intrinsic advantages. However, MoSe2 still encounters the issues of structural instability and poor rate performance caused by drastic volume change and sluggish reaction kinetics. Reasonable design of electrode structure is crucial for achieving superior electrochemical performance. Herein, a novel hierarchical structure coupled with 1D/1D subunits is elaborately designed and constructed, in which the MoSe2/CoSe2 heterostructure is the “trunk” and the N-doped carbon nanotubes are the “branches” (MoSe2/CoSe2/NCNTs). Benefiting from the properties endowed by unique configurations, MoSe2/CoSe2/NCNTs electrodes manifest faster reaction kinetics and better structure durability. Evaluated as an anode for LIBs and SIBs, MoSe2/CoSe2/NCNTs deliver high reversible capacity, superior rate capability (452 at 10 A g−1 in LIBs and 296 at 10 A g−1 in SIBs), and prominent cycle life (553 after 2000 cycles at 5 A g−1 in LIBs and 310 after 2000 cycles at 5 A g−1 in SIBs). Such design conception can also provide guidance for the development of other high-performance electrodes.

Layer effects on MXenes electrode and it applied to silicon composite structures

Despite the very high capacity of Si (4200mAh g−1), the widespread application of Si anodes has been hampered by drastic volume changes (up to 300 %) during cycling, leading to electrical contact losses and thus a sharp drop in capacity as the cycle life is shortened. Here we present a class of layered MXene/Si electrodes, which consist of nano-Si embedded in the interlayers of MXene to form a coupling effect, which can inhibit the huge volume change of Si during cycling. Therefore, layered MXene/Si has a highly reversible capacity, much improved cycling performance and excellent mechanical properties. First-principles calculations reveal the excellent electronic conductivity and good diffusion ability of layered MXene/Si, confirming the rapid storage of Li ions. This study provides useful information for the development and production of anode materials with high energy density and good mechanical properties.

In Situ Integration of a Flame Retardant Quasisolid Gel Polymer Electrolyte with a Si-Based Anode for High-Energy Li-Ion Batteries.

Silicon (Si) stands out as a promising high-capacity anode material for high-energy Li-ion batteries. However, a drastic volume change of Si during cycling leads to the electrode structure collapse and interfacial stability degradation. Herein, a multifunctional quasisolid gel polymer electrolyte (QSGPE) is designed, which is synthesized through the in situ polymerization of methylene bis(acrylamide) with silica-nanoresin composed of nanosilica and a trifunctional cross-linker in cells, leading to the creation of a "breathing" three-dimensional elastic Li-ion conducting framework that seamlessly integrates an electrode, a binder, and an electrolyte. The silicon particles within the anode are encapsulated by buffering the QSGPE after cross-linking polymerization, which synergistically interacts with the existing PAA binder to reinforce the electrode structure and stabilize the interface. In addition, the formation of the LiF- and Li3N-rich SEI layer further improves the interfacial property. The QSGPE demonstrates a wide electrochemical window until 5.5 V, good flame retardancy, high ionic conductivity (1.13 × 10-3 S cm-1), and a Li+ transference number of 0.649. The advanced QSGPE and cell design endow both nano- and submicrosized silicon (smSi) anodes with high initial Coulombic efficiencies over 88.0% and impressive cycling stability up to 600 cycles at 1 A g-1. Furthermore, the NCM811//Si cell achieves capacity retention of ca. 82% after 100 cycles at 0.5 A g-1. This work provides an effective strategy for extending the cycling life of the Si anode and constructing an integrated cell structure by in situ polymerization of the quasisolid gel polymer electrolyte.

Enhanced Silicon Anodes with Robust SEI Formation Enabled by Functional Conductive Binder

AbstractThe application of silicon (Si) anode is limited by the drastic volume change of silicon in the lithiation/delithiation process, the repeated formation of the solid electrolyte interface (SEI), and the low intrinsic conductivity. In this work, a small amount of poly (3,4‐ethylenedioxythiophene):poly (styrene sulfonic acid) (PEDOT:PSS) (PP), citric acid (CA), isopropyl alcohol (IPA), and silicon nanoparticles (SiNPs) are mixed and vacuum treated at a specific temperature to obtain silicon‐based anode electrode composite Si@PP@CA. The interphase forms a robust elastic network with hydrogen and chemical bonds, which have good mechanical properties and self‐repairing characteristics. The modified PEDOT:PSS as the conductive medium significantly improves the charge transfer rate. Moreover, the rapid formation of SEI by CA on the surface of SiNPs enhances the structural stability of the material. The electrochemical results show that the capacity of Si@PP@CA composite electrode canretain more than 2200 mAh g−1 after 200 cycles at 0.2 A g−1. It still shows a high capacity retention of 89% even at the current density of 1.0 A g−1 after 2000 cycles. More importantly, such excellent performance can be obtained using an electrode with an active material content of up to 90 wt%, which is essential for practical applications.

Realization of high-capacity coulombic efficiency in sodium alginate/carbon nanotube double network coated Si-anode for lithium-ion batteries

Silicon (Si) is considered as one of the most promising anodes for the next-generation lithium-ion batteries (LIBs) owing to its ultra-high specific capacity, low redox potential and the second abundance of elements in the earth's crust. However, drastic volume change will directly cause electrode pulverization, thus leading to low initial coulombic efficiency (ICE) and terrible cycling stability. In this work, a sodium alginate (SA)‑carbon nanotube (CNT) derived double carbon-coated Si composite (SA-CNT@Si) was prepared through freeze-drying technique followed by high-temperature carbonization, where SA was utilized to encase Si nanospheres, with CNT serving as the conductive framework that interconnects Si spheres. These composites exhibit improved electrical conductivity and stability throughout the charge and discharge cycles when employed as the anodes in LIBs, demonstrating superior electrochemical properties. The SA-CNT@Si electrode with a mass ratio of Si: SA: CNT = 5: 1: 0.75, achieved a first discharge specific capacity of 2200.8 mAh g−1 at a current density of 500 mA g−1 (with the initial three cycles at 100 mA g−1), along with an ICE of 86.2%. Even after 500 cycles, it maintained a capacity of 607 mAh g−1. This study presents a novel approach to designing Si-based anode materials characterized by both high electrical conductivity and structural stability.

Reduced Volume Expansion of Micron-Sized SiOx via Closed-Nanopore Structure Constructed by Mg-Induced Elemental Segregation.

The inherently huge volume expansion during Li uptake has hindered the use of Si-based anodes in high-energy lithium-ion batteries. While some pore-forming and nano-architecting strategies show promises to effectively buffer the volume change, other parameters essential for practical electrode fabrication, such as compaction density, are often compromised. Here we propose a new in situ Mg doping strategy to form closed-nanopore structure into a micron-sized SiOx particle at a high bulk density. The doped Mg atoms promote the segregation of O, so that high-density magnesium silicates form to generate closed nanopores. By altering the mass content of Mg dopant, the average radii (ranged from 5.4 to 9.7 nm) and porosities (ranged from 1.4 % to 15.9 %) of the closed pores are precisely adjustable, which accounts for volume expansion of SiOx from 77.8 % to 22.2 % at the minimum. Benefited from the small volume variation, the Mg-doped micron-SiOx anode demonstrates improved Li storage performance towards realization of a 700-(dis)charge-cycle, 11-Ah-pouch-type cell at a capacity retention of >80 %. This work offers insights into reasonable design of the internal structure of micron-sized SiOx and other materials that undergo conversion or alloying reactions with drastic volume change, to enable high-energy batteries with stable electrochemistry.

Reduced Volume Expansion of Micron‐Sized SiOx via Closed‐Nanopore Structure Constructed by Mg‐Induced Elemental Segregation

AbstractThe inherently huge volume expansion during Li uptake has hindered the use of Si‐based anodes in high‐energy lithium‐ion batteries. While some pore‐forming and nano‐architecting strategies show promises to effectively buffer the volume change, other parameters essential for practical electrode fabrication, such as compaction density, are often compromised. Here we propose a new in situ Mg doping strategy to form closed‐nanopore structure into a micron‐sized SiOx particle at a high bulk density. The doped Mg atoms promote the segregation of O, so that high‐density magnesium silicates form to generate closed nanopores. By altering the mass content of Mg dopant, the average radii (ranged from 5.4 to 9.7 nm) and porosities (ranged from 1.4 % to 15.9 %) of the closed pores are precisely adjustable, which accounts for volume expansion of SiOx from 77.8 % to 22.2 % at the minimum. Benefited from the small volume variation, the Mg‐doped micron‐SiOx anode demonstrates improved Li storage performance towards realization of a 700‐(dis)charge‐cycle, 11‐Ah‐pouch‐type cell at a capacity retention of >80 %. This work offers insights into reasonable design of the internal structure of micron‐sized SiOx and other materials that undergo conversion or alloying reactions with drastic volume change, to enable high‐energy batteries with stable electrochemistry.

In situ atomic-scale tracking of unusual interface reaction circulation and phase reversibility in (de)potassiated alloy-typed anode

Alloy-typed anode materials, endowed innately with high theoretical specific capacity, hold great promise as an alternative to intercalation-typed counterparts for alkali-ion batteries. Despite tremendous efforts devoted to addressing drastic volume change and severe pulverization issues of such anodes, the underlying mechanisms involving dynamic phase evolutions and reaction kinetics have not yet been fully comprehended. Herein, taking antimony (Sb) anode as a representative paradigm, its microscopic operating mechanisms down to the atomic scale during live (de)potassiation cycling are systematically unraveled using in situ transmission electron microscopy. Highly reversible phase transformations at single-particle level, that are Sb ↔ KSb2 ↔ KSb ↔ K5Sb4 ↔ K3Sb, were revealed during cycling. Meanwhile, multiple phase interfaces associated with different reaction kinetics coexisted and this phenomenon was properly elucidated in the context of density functional theory calculations. Impressively, previously unexplored unidirectional circulation of reaction interfaces within individual Sb particle is confirmed for both potassiation and depotassiation. Based on the empirical results, the surface diffusion-mediated potassiation-depotassiation pathways at single-particle level are suggested. This work affords new insights into energy storage mechanisms of Sb anode and valuable guidance for targeted optimization of alloy-typed anodes (not limited to Sb) toward advanced potassium-ion batteries.

Pomegranate-like heterostructured SnS2/CoS2 particles encapsulated in S, N dual-doped carbon framework enabling high-rate and durable sodium ion storage

As a promising anode material for sodium-ion batteries, SnS2 has attracted increasing attention owing to its high theoretical capacity and abundant reserves. Unfortunately, the poor electrical conductivity and drastic volume changes lead to unsatisfactory cycling and rate performance, largely limiting its practical application. Herein, we report a pomegranate-like composite of heterostructured SnS2/CoS2 spheres encapsulated in S, N dual-doped carbon framework (SnS2/CoS2@SNC) obtained by a simple ion adsorption, in situ polymerization coating of polydopamine and subsequent calcination strategy. The integration of CoS2 with SnS2 particles with abundant interfaces can provide rich redox chemistry and accelerated ion diffusion kinetics, while the coated S, N dual-doped carbon shell enables good electrical conductivity and reinforced structural integrity as well by accommodating the volume changes and inhibiting the collapse/pulverization of active materials during the cycling process. As a consequence, the pomegranate-like heterostructured SnS2/CoS2@SNC anode exhibited a higher capacity (743 mAh g−1 at 1 A g−1), excellent rate capability (213 mAh g−1 at 50 A g−1) and outstanding cycling stability (560 mAh g−1 at 5 A g−1 after 1000 cycles), showing the application feasibility of this anode material for developing high-rate and durable SIBs.

Deciphering Unexplored Reversible Potassium Storage and Small Volume Change in a CaV4O9 Anode with In Situ Transmission Electron Microscopy

AbstractVanadium‐based compounds are explored as promising electrode materials in lithium/sodium‐ion batteries exhibiting superior energy storage properties. However, similar attempts are rarely reported for potassium‐ion batteries (PIBs), in which the fundamental reaction mechanisms remain inexplicit. Herein, porous CaV4O9 nanobelts (NBs) are selected as a PIB anode to systematically investigate potassium storage mechanisms through in situ transmission electron microscopy. In situ measurements track overall electrochemical potassiation reactions of CaV4O9 and identify a polyphase state of V4O7, CaO, and K2O phases after potassiation. Unexpectedly, the potassiated products can be partially converted back to the original CaV4O9 phase with residual VO2 and CaO phases, which is different from the irreversible phase transformations in lithium/sodium storages of CaV4O9. Impressively, the cavities in NBs alternately disappear and appear with (de)potassiation, avoiding the drastic volume change and structural degradation of anodes. The reversible potassium storage and stable cycling are evaluated by electrochemical measurements and in situ X‐ray diffraction analysis. This work provides a paradigm by revisiting the existing anode materials in lithium/sodium‐ion batteries to seek out viable anodes for next‐generation PIBs.

Improving Structural and Chemical Stability of O3-Type Sodium Layered Oxide Cathode Via Fluorination

A spherical O3-type layered oxide cathode, composed of compactly‐packed nanosized primary particles, is synthesized by the coprecipitation method so that the high tap density of the cathode ensures increased volumetric energy density for energy storage applications. However, drastic volume changes in the deeply charged states contribute to structural degradation, by inducing mechanical stress and the eventual disintegration of the cathode particles by the formation of microcrack. The microcrack traversing the entire secondary particle compromise the mechanical integrity of the cathode and accelerate electrolyte infiltration into the particle interior, causing the subsequent degradation of the exposed internal surfaces. In this study, we suggested a promising fluorination strategy to extend the cycle life of the O3‐type Na[Ni0.5Mn0.5]O2 cathode by improving their mechanical integrity and protecting their surfaces against electrolyte attack. Fluorination not only inhibits the microcracking of cathode secondary particles but also suppresses surface degradation, i.e., the formation of an electrochemically inactive NiO-like rock salt phase and dissolution of transition metals into electrolyte solution.

Facile Synthesis of 2D SiOx-3D Si Hybrid Anode Materials by Ca Modification Effect for Enhanced Lithium Storage Performance.

Al-Si dealloying method is widely used to prepare Si anode for alleviating the issues caused by a drastic volume change of Si-based anode. However, this method suffers from the problems of low Si powder yield (<20wt.% Si) and complicated cooling equipment due to the hindrance of large-size primary Si particles. Here, a new modification strategy to convert primary Si to 2D SiOx nanosheets by introducing a Ca modifier into Al-Si alloy melt is presented. The thermodynamics calculation shows that the primary Si is preferentially converted to CaAl2Si2 intermetallic compound in Al-Si-Ca alloy system. After the dealloying process, the CaAl2Si2 is further converted to 2D SiOx nanosheets, and eutectic Si is converted to 3D Si, thus obtaining the 2D SiOx-3D Si hybrid Si-based materials (HSiBM). Benefiting from the modification effect, the HSiBM anode shows a significantly improved electrochemical performance, which delivers a capacity retention of over 90% after 100 cycles and keeps 98.94% capacity after the rate test. This work exhibits an innovative approach to produce stable Si-based anode through Al-Si dealloying method with a high Si yield and without complicated rapid cooling techniques, which has a certain significance for the scalable production of Si-based anodes.

A Room-Temperature Self-Healing Liquid Metal-Infilled Microcapsule Driven by Coaxial Flow Focusing for High-Performance Lithium-Ion Battery Anode.

Liquid metals have attracted a lot of attention as self-healing materials in many fields. However, their applications in secondary batteries are challenged by electrode failure and side reactions due to the drastic volume changes during the "liquid-solid-liquid" transition. Herein, a simple encapsulated, mass-producible method is developed to prepare room-temperature liquid metal-infilled microcapsules (LMMs) with highly conductive carbon shells as anodes for lithium-ion batteries. Due to the reasonably designed voids in the microcapsule, the liquid metal particles (LMPs) can expand freely without damaging the electrode structure. The LMMs-based anodes exhibit superior capacity of rete-performance and ultra-long cycling stability remaining 413mAhg-1 after 5000 cycles at 5.0Ag-1. Ex situ X-ray powder diffraction (XRD) patterns and electrochemical impedance spectroscopy (EIS) reveal that the LMMs anode displays a stable alloying/de-alloying mechanism. DFT calculations validate the electronic structure and stability of the room-temperature LMMs system. These findings will bring some new opportunities to develop high-performance battery systems.