Li-ion Diffusion Research Articles

3D Cu Pyramid Array Grown on Planar Cu Foil for Stable and Dendrite-free Lithium Deposition

Lithium metal is recognized as the anticipated anode for rechargeable batteries because of its inherent physicochemical properties. Unfortunately, the industrialization of Li metal anodes (LMAs) has been entangled in some intractable problems stemming from the uncontrollable growth of Li dendrites, which could result in the issue of short-circuit, thereby leading to cell failure. Here, a three-dimensional structured Cu pyramid array (CPA@CF) is constructed on planar Cu foil (CF) by the simple electrodeposition method. Owing to the features of large surface area and 3D porous structure, the proposed CPA@CF not only can promote Li-ion diffusion and charge transfer, but also effectively slow down the volume change of Li. Consequently, an even and steady Li plating/stripping process up to 360 h is realized using such a CPA@CF current collector. The Li@CPA@CF|LiFePO4 full cell achieves an excellent Coulombic efficiency (CE) of 99.3 % for 160 cycles at 0.3 C with a superior capacity retention of 84.2 %.

Research progress in solid-state synthesized LiMnPO4 cathode material for Li-ion battery applications

LiMnPO4 cathode material and its derivatives are promising for energy-storage devices owing to its environmental friendliness, high energy density, and structural stability. Olivine LiMnPO4 is attractive due to its high operating voltage (4 to 5 V vs. Li+/Li), and strong P-O covalent bond, which offers many safety advantages. Despite these advantages, the commercialization of LiMnPO4-based lithium-ion batteries (LIB) has been plagued by other factors such as poor electronic and ionic conductivity, a high surface energy barrier for Li-ion diffusion, and structural degradation induced by the Jahn-Teller effect. Various strategies, including transition metal doping at the A-site and the fabrication of heterostructures with high electron mobility, have been employed to address these challenges. Notably, the exceptional electrode performance of microrods may be ascribed to their distinct three-dimensional porous hierarchical structure, which promotes rapid Li+ transport kinetics and improves structural stability in reversible electrochemical reactions. While these enhancement techniques are centered on processing, solid-state chemistry is more effective, offering convenience in overcoming obstacles related to physiochemical and electrochemical performance. The solid-state synthesis approach, typically known for its capability to tailor the size and morphology of materials, has demonstrated a significant impact on enhancing the electrochemical activity of LiMnPO4. This review critically discusses the structure dependence of LiMnPO4 cathode material on electrochemical reactions. It gives a broad overview of the research approaches being employed to enhance the structure and electrochemical performance of LiMnPO4 through the solid-state technique. It also provides a comprehensive overview of the challenges and the need for further research to fully realize the potential of LiMnPO4 cathodes as a promising cathode material for Li-Ion batteries.

Lithium disilicate as an alternative silicate battery material. A theoretical study

Advanced atomistic simulations are used to study the ion transport in the Na- and K-doped lithium disilicate Li2Si2O5 which is considered as a potential battery material for solid state alkali batteries. In order to evaluate the ease with which Li2Si2O5 can store Na and K ions, the Na and K incorporation mechanisms into Li2Si2O5 are studied by using lattice statics simulations. Our calculations revealed that the defect formation energies for K and Na doping of Li2Si2O5 amount to 0.49 eV/dopant and 0.96 eV/dopant, respectively. The Li ion diffusion in Li2Si2O5 is significantly enhanced upon Na and K doping. The activation energies of Li ion diffusion in all samples are in the range of 0.5–0.6 eV, while for conduction 0.4–0.5 eV. At higher dopant concentrations, K doping increases the Li ion diffusion/conduction, reaching their improved transport properties at x = 0.14 with low activation energy for diffusion and conduction. At a low dopant concentration of x = 0.02, Na doping also improves the Li ion diffusion/conduction. Our results demonstrate the potential of the doped lithoum disilicate Li2Si2O5 as an effective material for alkali ion batteries and strongly suggest experimental verification.

A Promising Solid-State Synthesis of LiMn1- yFeyPO4 Cathode for Lithium-ion Batteries.

LiMn1-yFeyPO4 (LMFP) is a significant and cost-effective cathode material for Li-ion batteries, with a higher working voltage than LiFePO4 (LFP) and improved safety features compared to layered oxide cathodes. However, its commercial application faces challenges due to a need for a synthesis process to overcome the low Li-ion diffusion kinetics and complex phase transitions. Herein, a solid-state synthesis process using LFP and nano LiMn0.7Fe0.3PO4 (MF73) is proposed. The larger LFP acts as a structural framework fused with nano-MF73, preserving the morphology and high performance of LFP. These results demonstrate that the solid-state reaction occurs quickly, even at a low sintering temperature of 500 °C, and completes at 700 °C. However, contrary to the expectations, the larger LFP particles disappeared and fused into the nano-MF73 particles, revealing that Fe ions diffuse more easily than Mn ions in the olivine framework. This discovery provides valuable insights into understanding ion diffusion in LMFP. Notably, the obtained LMFP can still deliver an initial capacity of 142.3 mAh g-1, and the phase separation during the electrochemical process is significantly suppressed, resulting in good cycling stability (91.1% capacity retention after 300 cycles). These findings offer a promising approach for synthesizing LMFP with improved performance and stability.

Unlocking the Potential of Li-Rich Mn-Based Oxides for High-Rate Rechargeable Lithium-Ion Batteries.

Lithium-rich Mn-based oxides have gained significant attention worldwide as potential cathode materials for the next generation of high-energy density lithium-ion batteries. Nonetheless, the inferior rate capability and voltage decay issues present formidable challenges. Here, a Li-rich material equipped with quasi-three-dimensional (quasi-3D)Li-ion diffusion channels is initially synthesized by introducing twin structures with high Li-ion diffusion coefficients into the crystal and constructing a "bridge" between different Li-ion diffusion tunnels. The as-prepared material exhibits monodispersed micron-sized primary particles (MP), delivering a specific capacity of 303mAhg-1 at 0.1 C and an impressive capacity of 253mAhg-1 at 1 C. More importantly, the twin structure also serves as a "breakwater" to inhibit the migration of Mn ions and improve the overall structural stability, leading to cycling stability with 85% capacity retention at 1 Cafter 200 cycles. The proposed strategy of constructing quasi-3Dchannels in the layered Li-rich cathodes will open up new avenues for the research and development of other layered oxide cathodes, with potential applications in industry.

Promoting homogeneous lithiation of silicon anodes via the application of bifunctional PEDOT:PSS/PEG composite binders

Polymeric conducting binders have increasingly become a subject of significant research interest due to their dual roles as both a binder and a conducting agent. This dual functionality not only increases the proportion of active materials in the electrode but also elevates the volumetric energy density of current Li-ion batteries. In this study, we explore the potential of a composite of PEDOT:PSS and polyethylene glycol (PEG) as a high-performing binder for silicon anodes. This highly conductive PEDOT:PSS, enhanced by the addition of PEG polymer, displays exceptional electrochemical characteristics, including superior C-rate, Li-ion diffusivity performance, and extended cycle endurance. Of particular interest are the enhanced mechanical properties bestowed by the plasticizing effect of the PEG polymer. This improvement aids the Si anode in resisting pulverization during successive discharge and charge cycles. As a result, this enables extended cyclability without the creation of anode cracking. Additionally, the use of operando optical microscopy allows for the direct observation of lithiation kinetics within the PEDOT:PSS/PEG binder. This revealed a uniform color change with restrained volume expansion, demonstrating the successful operation of the binder. Consequently, the bifunctional PEDOT:PSS/PEG binder shows promise as a robust strategy for the next generation of high-performance lithium-ion battery binders.

A permselective protection layer assembled by two-dimensional organic vermiculite produces a highly stable lithium metal anode for lithium-sulfur batteries

Designing a protective coating for the lithium metal anode is the crucial yet challenging solution to its practical applications. How to well isolate the reactants in electrolytes but allow fast and uniform ion diffusion is the greatest challenge for various high energy density batteries, e.g., lithium–sulfur batteries. Herein, we propose a permselective protect coating, which has the ability to accelerate the homogeneous fast Li-ion diffusion but block the polysulfide anion penetration, and obtain a dendrite-free and corrosion-resistive lithium metal anode. The above ion-sieving function is realized by a membrane assembled with cetyltrimethylammonium (CTA+)-modified two-dimensional organic vermiculite nanosheets. The enlarged interlayer spacing of the membrane with CTA+ and the negative charges on the vermiculite nanosheets enhance the fast Li-ion transmission across the membrane for uniform Li deposition. At the same time, the non-polar alkyl of CTA+ and the negatively charged surface effectively block the polysulfide adsorption and penetration. Therefore, the side reactions and dendrite growth are effectively suppressed, and with the high sulfur loading (5 mg/cm2) and limited E/S ratio, the assembled lithium–sulfur cell shows good cycling stability at 0.1C, revealing a high capacity retention of 65.9 % over 300 cycles.

Strain effects on [formula omitted] anti-perovskite solid lithium-ion electrolytes: DFT study

We have systematically explored the impact of strain on various properties of Li3OX(X=Cl,Br) anti-perovskite solid lithium-ion electrolytes based on the density functional theory. The responses of bandgap, defect formation energy, Li-ion migration barrier energy and diffusivity were discussed under different strain conditions, encompassing isotropic and biaxial compressive/tensile strains ranging from −4% to 4%. Our results reveal intriguing insights: Tensile strain leads to a substantial reduction in the bandgap by up to 0.5 eV, whereas for Li3OCl/Br under compressive strain, the reduction is only ∼0.1 eV. Additionally, tensile strain facilitates the formation of Li+ vacancies and Li interstitials, thereby promoting the Li-ion diffusivity. Furthermore, the Li-ion migration barrier energy decreases when tensile strain is applied along the O–Li–O distribution direction. Analysis of AIMD results shows that tensile strain effectively enhances the diffusivity of Li ions. These findings suggest that isotropic strain strongly affects Li-ion conductivities in Li3OCl/Br anti-perovskite electrolytes, and applying tensile strain can be a potential method to enhance lithium transport.

Soy protein isolate/MXene decorated acidified carbon paper interlayer for long‐cycling Li–S batteries

AbstractThe terrible shuttling of lithium polysulfides (LiPSs) is a major obstacle for commercializing lithium–sulfur (Li–S) batteries as high‐performance energy storage systems. In this study, a carbon‐based interlayer with effective suppression capability on the shuttle effect is developed by simply coating a well‐dispersed mixture of soybean protein isolate/MXene onto the acidified carbon paper (ACP). The resultant composite interlayer (SM@ACP) is able to synergistically diminish the shuttle effect through chemical adsorption and physical blocking. Meanwhile, this interlayer displays excellent conductivity and facilitates the diffusion of Li ions due to the composite coating to promote both electron/ion conduction as well as the porous structure of ACP. Benefiting from the unique properties of the composite interlayer, the as‐assembled Li–S batteries with SM@ACP interlayers show a great improvement in the cycling stability and rate performance, delivering a very low‐capacity decay rate of 0.071% per cycle at 0.5 C even after 800 cycles. This work provides a feasible route to realize rational design and commercial mass production of desirable interlayers for promoting the commercialization of Li–S batteries.

First-Principles Study on the Interplay of Strain and State-of-Charge with Li-Ion Diffusion in the Battery Cathode Material LiCoO2.

Cathode degradation of Li-ion batteries (Li+) continues to be a crucial issue for higher energy density. A main cause of this degradation is strain due to stress induced by structural changes according to the state-of-charge (SOC). Moreover, in solid-state batteries, a mismatch between incompatible cathode/electrolyte interfaces also generates a strain effect. In this respect, understanding the effects of the mechanical/elastic phenomena associated with SOC on the cathode performance, such as voltage and Li+ diffusion, is essential. In this work, we focused on LiCoO2 (LCO), a representative LIB cathode material, and investigated the effects of biaxial strain and hydrostatic pressure on its layered structure and Li+ transport properties through first-principles calculations. With the nudged elastic band technique and molecular dynamics, we demonstrated that in Li-deficient LCO, compressive biaxial strain increases the Li+ diffusivity, whereas tensile biaxial strain and hydrostatic pressure tend to suppress it. Structural parameter analysis revealed the key correlation of "Co layer distances" with Li+ diffusion instead of "Li layer distances", as ordinarily expected. Structural analysis further revealed the interplay between the Li-Li Coulomb interaction, SOC, and Li+ diffusion in LCO. The activation volume of LCO under hydrostatic pressure was reported for the first time. Moreover, vacancy formation energy calculations showed that the Li intercalation potential could be decreased under compressive biaxial strain due to the weakening of the Li-O bond interaction. The present findings may serve to improve the control of the energy density performance of layered cathode materials.

Pyrochlore-Type Iron Hydroxy Fluorides as Low-Cost Lithium-Ion Cathode Materials for Stationary Energy Storage.

Pyrochlore-type iron (III) hydroxy fluorides (Pyr-IHF) are appealing low-cost stationary energy storage materials due to the virtually unlimited supply of their constituent elements, their high energy densities and fast Li-ion diffusion. However, the prohibitively high cost of synthesis and cathode architecture currently prevent their commercial use in low-cost Li-ion batteries. Herein, we present a facile and cost-effective dissolution-precipitation synthesis of Pyr-IHF from soluble iron (III) fluoride precursors. High capacity retention by synthesized Pyr-IHF of > 80% after 600cycles at a high current density of 1Ag-1 was obtained, without elaborate electrode engineering. Operando synchrotron X-ray diffraction guided the selective synthesis of Pyr-IHF such that different water contents could be tested for their effect on the rate capability. Li-ion diffusion was found to occur in the 3D hexagonal channels of Pyr-IHF, formed by corner-sharing FeF6-x (OH)x octahedra. This article is protected by copyright. All rights reserved.

Insights into the kinetics–morphology relationship of 1-, 2-, and 3D TiNb2O7 anodes for Li-ion storage

Understanding the influence of electrode material’s morphology on electrochemical behavior is of great significance for the development of rechargeable batteries, however, such studies are often limited by the inability to precisely control the morphology of electrode materials. Herein, nanostructured titanium niobium oxides (TiNb2O7) with three different morphologies (one-dimensional (1D), two-dimensional (2D), and three-dimensional (3D)) were synthesized via a facile microwave-assisted solvothermal method. The influence of the morphological dimension of TiNb2O7 as electrode material on the electrochemical performance in Li-ion batteries (LIBs) and the underlying correlation with the electrochemical kinetics were studied in detail. 2D TiNb2O7 (TNO-2D) shows a superior rate capability and cycling stability, associated with improved kinetics for charge transfer and Li-ion diffusion, compared to the 1D and 3D materials. Operando X-ray diffraction measurements reveal the structural stability and crystallographic evolution of TNO-2D upon lithiation and delithiation and correlate the Li-ion diffusion kinetics with the lattice evolution during battery charge and discharge. Moreover, carbon-coated TNO-2D achieves enhanced rate capability (205 mAh·g−1 at 50 C) and long-term cycling stability (87% after 1000 cycles at 5 C). This work provides insights into the rational morphology design of electrode materials for accelerated charge transfer and enhanced fast-charging capability, pushing forward the development of electrode materials for high-power rechargeable batteries in future energy storage.

Effects of High Hydrostatic Pressure on the Structural, Electronic, and Elastic Properties, and Li-Ion Diffusion Barrier of Lithium Lanthanum Titanate Electrolytes: A DFT Study

Lithium lanthanum titanate perovskites (LLTO) are excellent solid electrolytes because of their good ionic conductivity and elasticity. In this work, the effects of high hydrostatic pressure and the impact of the position of Li impurities on the structural, electronic, elastic, and Li-ion diffusion properties of LaTiO3 perovskite (LTO) and its LLTO substitutional solid solutions, were studied. Density-Functional Theory (DFT) and Hubbard-corrected Local Density Approximation (LDA+U) were used. Due to hydrostatic pressure, the octahedral distortion of LTO, LLTO-layered (L), and -rock-salt (RS) electrolytes decreases, while it increases for the LLTO-columnar (C). On the other hand, the energy band gap () of LTO and LLTO-C decrease as hydrostatic pressure increases. For the LLTO-L, increases with pressure. For the LLTO-RS, decreases from zero to 20 GPa and increases from 20 to 30 GPa. Pugh’s criterion indicates that all systems are ductile regardless of applied pressure. Poisson’s ratio shows that bonds in the LTO are metallic, and LLTO-C is ionic-covalent. Likewise, LLTO-L and -RS electrolytes have a transition from ionic-covalent to metallic behavior, as pressure increases. Li-ion diffusion barriers of LLTO electrolytes increase with increasing hydrostatic pressure, indicating a decrease in Li ionic conductivity.

Tailored synthesis of NdMnxFe1-xO3 perovskite nanoparticles with oxygen-vacancy defects for lithium-ion battery anodes

In this study, we synthesize nanostructured NdMnxFe1-xO3 perovskites using a facile method to produce materials for the high-working-efficiency anodes of Li-ion batteries. A series of characterization assessments (e.g., X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and electron microscopy) were conducted, and the results confirmed the efficacious partial replacement of Fe ions with Mn ions in the NdFeO3 perovskite structure, occurrence of both amorphous and crystalline structures, presence of oxygen vacancies (VO), and interconnection between nanoparticles. The possibility of Mn ion replacement significantly affects the size, amount of VO, and ratio of amorphous phase in NdMnxFe1-xO3 perovskites. The NdMnxFe1-xO3 perovskite with x = 0.3 presents a notable electrochemical performance, including low charge transfer resistance, durable Coulombic efficiency, first-rate capacity reservation, high pseudo-behavior, and elongated 150-cycle service life, whereas no discernible capacity deterioration is observed. The reversible capacity of the anode after the 150th-cylcle was 713 mAh g−1, which represents a high-capacity value. The outstanding electrochemical efficiency resulted from the optimum presence of VO, interconnection between the nanoparticles, and distinctive properties of the NdFeO3 perovskite. The interconnection between nanoparticles was advantageous for forming a large electrolyte-electrode contact area, improving Li-ion diffusion rates, and enhancing pseudocapacitive effect. The attributes of perovskite crystals, coexistence of Mn and Fe throughout the charge/discharge process, and optimum VO precluded the electrode devastation that caused the Li2O-phase decomposition catalysis, enabling favorable reversible Li storage.

Unlocking the potential of silicon anodes in lithium-ion batteries: A claw-inspired binder with synergistic interface bonding

Binders play a crucial role in enhancing the cycling stability of silicon anodes in next-generation Li-ion batteries. However, traditional linear polymer binders have difficulty withstanding the volume expansion of silicon during cycling. Herein, inspired by the fact that animals’ claws can grasp objects firmly, a claw-like taurine-grafted-poly (acrylic acid) binder (Tau-g-PAA) is designed to improve the electrochemical performance of silicon anodes. The synergistic effects of different polar groups (sulfo and carboxyl) in Tau-g-PAA facilitate the formation of multidimensional interactions with silicon nanoparticles and the diffusion of Li ions, thereby greatly improving the stability and rate performance of silicon anodes, which aligns with results from density functional theory (DFT) simulations. As expected, a Tau-g-PAA/Si electrode exhibits excellent cycling performance with a high specific capacity of 1003 ​mA ​h ​g−1 ​at 1 ​C (1 ​C ​= ​4200 ​mA ​h ​g−1) after 300 cycles, and a high rate performance. The design strategy of using polar small molecule-grafted polymers to create claw-like structures could inspire the development of better binders for silicon-based anodes.

Effect of concentration-driven magnetic phase changes on adsorption and diffusion in VSe2 monolayers: Implications for lithium-ion batteries

A vanadium diselenide (VSe2) monolayer is a two-dimensional (2D) magnetic material that exhibits ferromagnetic ordering at room temperature and exceptional metal-ion storage capacity, making it useful in spintronics and energy storage applications. However, a robust correlation between the magnetic and electrochemical properties of VSe2 remains to be established. In this study, first-principles density functional theory calculations were performed to investigate the effect of increasing Li-ion concentrations on the magnetic properties, particularly the magnetic ground state of the VSe2 monolayer. The results indicate that, as the concentration of Li ions on the surface of VSe2 monolayer increases, magnetic phase transitions occur, leading to a shift from the intrinsic ferromagnetic (FM) state to antiferromagnetic (AFM) and non-magnetic ground states. Analyses of the diffusion properties of ferromagnetic and antiferromagnetic VSe2 monolayers revealed a considerable (∼71%) increase in the Li-ion diffusion energy barrier for the AFM state compared to the FM state. This implies that FM-VSe2 facilitates relatively faster diffusion of Li ions than AFM-VSe2. Therefore, the Li-ion concentration-induced phase change in the VSe2 monolayer leads to variable adsorption and diffusion characteristics, which will have significant implications for its use in Li-ion battery anodes.

Bidirectional redox catalyst with rambutan-like structure for advanced lithium-sulfur battery

The lithium polysulfide (LiPSs) shuttle effect and sluggish conversion kinetics hinder the commercial viability of lithium-sulfur (Li-S) batteries. To improve the properties of Li-S batteries, it is imperative to establish efficient pathways for Li-ions transmission by constructing conductivity channels of high quality, and to expedite the conversion kinetics of LiPSs by employing catalysts of exceptional activity. In this study, we synthesized a spherical superstructure of metal–organic framework nanorods (SS-MOFNR) using a self-assembly strategy with zinc-metal–organic framework (Zn-MOF) nanoparticles, followed by carbonization to obtain the spherical superstructure of carbon nanorods (SS-CNR). Subsequently, palladium nanoparticles were synthesized through the reduction and uniformly dispersed onto SS-CNR. The hollow porous structure facilitates the efficient utilization of sulfur and ensures the rapid diffusion of Li-ions. Additionally, Pd nanoparticles exhibit significant catalytic activity, effectively adsorbing LiPSs and bidirectional catalytic conversion of sulfur species, thereby effectively suppressing the shuttle effect of LiPSs. Therefore S/Pd@SS-CNR electrode demonstrates commendable electrochemical efficacy, as evidenced by its initial specific capacity of 1627.7 mAh g−1 at 0.1C and maintaining a specific capacity of 766.2 mAh g−1 even after 600 cycles at 0.5C. Moreover, it exhibits favorable cycle stability at 2C, retaining a reversible capacity of 502.3 mAh g−1 after undergoing 1000 cycles.

Surface morphology engineering of WO3 films for increasing Li ion insertion area in electrochromic supercapacitors (ECSCs)

Two different dry deposition methods were used to deposit electrode films with different surface morphologies in relation to the performance of electrochromic supercapacitors (ECSCs): direct current (DC) magnetron sputtering and the nanoparticle deposition system (NPDS). The NPDS method, which sprays powders onto the substrate using pressure differences, deposited WO3 film with its roughness of 36 nm and its thickness of 383 nm, while the sputtered WO3 film had its roughness of 3 nm and its thickness of 262 nm. Due to its dramatic difference in surface roughness, the NPDS-WO3 thin film had larger reaction surface area as well as Li-ion diffusion coefficient than those of sputtered-WO3 films. As a result, the ECSC device with NPDS-WO3 exhibited 19 % higher coloration efficiency with greater charge capacity compared to those with sputtered-WO3. However, the ECSC device with NPDS-WO3 showed different charge/discharge with trapped Li ions during the coloring(charging)/bleaching(discharge) processes respectively, leading to rapid degradation of the device. This research highlights the clear difference between its characteristics of the thin films fabricated using the NPDS vs. sputtering methods in relation to its surface roughness so that this study would be potentially beneficial in engineering various properties of ECSC devices.

Exploring the potential of one-dimensional van der Waals material V2PS10/carbon composite: An anode design paradigm for lithium-ion batteries

One-dimensional (1D) van der Waals (vdW) materials have garnered significant attention for their unique structures and properties, making them promising candidates for various applications in optoelectronics, catalysis, energy storage, and sensors. However, further advancements are required to fully exploit their potential as energy storage devices. This study presents an anode design paradigm utilizing 1D vdW-based V2PS10 crystals characterized by large vdW gaps, a small bandgap, and distinctive chemical compositions that favor lithium storage. To enhance their performance, we employ surface modification techniques to create V2PS10 @C composites, where conductive carbon is integrated with V2PS10 crystals. This modification significantly improves electron transport and Li-ion diffusion within the composite anodes. The resulting composite anodes exhibit exceptional electrochemical properties, including a high discharge capacity of 1154 mAh g−1 after the 50th cycle at 0.1 A g−1, superior rate performance with a current density of 561 mAh g−1 at 10 A g−1, and prolonged cycling stability, maintaining a capacity of 605 mAh g−1 for up to 800 cycles at 5 A g−1. These remarkable electrochemical performances underscore the immense potential of 1D vdW-based materials as next-generation anodes for lithium-ion batteries.

Rugby-ball-like Zinc molybdate electrodes for Li-ion battery anode applications

ZnMoO4 nanostructures with varying morphologies were synthesized using a simple hydrothermal technique, employing different Zn to Mo ratios. Various analytical techniques were employed to characterize both the structure and morphology of the ZnMoO4 nanostructures. As the Zn concentration in the reaction mixture was systematically increased, a transformation in morphology from non-uniform particles to uniform rugby-ball-like structures occurred. Additionally, there was a notable phase transition from predominantly α-ZnMoO4 phase to primarily β-ZnMoO4 phase. At a current density of 0.1 A g−1, the β-ZnMoO4 exhibited an initial discharge capacity of 2249 mAh g−1, while maintaining remarkable reverse rate capacity of 883 mAh g−1 even at a high current density of 0.2 A g−1. This uniform rugby-ball-like morphology favors Li-ion diffusion and ease of ion transfer from the electrode surface to electrolyte. The estimated gravimetric energy density LiCoO2//ZnMoO4 is 511 Wh kg−1, which is better than that of conventional LiCoO2//graphite (398 Wh kg−1). These findings underscore the exceptional properties of ZnMoO4, positioning it as a highly promising anode material for lithium-ion battery applications.