Ion Migration Barrier Research Articles

Boosting K+‐Ionic Conductivity of Layered Oxides via Regulating P2/P3 Heterogeneity and Reciprocity for Room‐Temperature Quasi‐Solid‐State Potassium Metal Batteries

AbstractSolid‐state potassium metal batteries are promising candidates for grid‐scale energy storage due to their low cost, high energy density and inherent safety. However, solid state K‐ion conductors struggle with poor ionic conductivity due to the large ionic radius of K+‐ions. Herein, we report precise regulation of phase heterogeneity and reciprocity of the P2/P3‐symbiosis K0.62Mg0.54Sb0.46O2 solid electrolyte (SE) for boosting a high ionic conductivity of 1.6×10−4 S cm−1 at 25 °C. The bulk ionic conducting mechanism is explored by elucidating the effect of atomic stacking mode within the layered framework on K+‐ion migration barriers. For ion diffusion at grain boundaries, the P2/P3 biphasic symbiosis property assists in tunning the SE microstructure, which crystallizes in rod‐like particles with lengths of tens of micrometers facilitating long‐distance ion transport and significantly decreasing grain boundary resistance. Potassium metal symmetric cells using the modified SE deliver excellent cycling life over 300 h at 0.1 mA cm−2 and a high critical current density of 0.68 mA cm−2. The quasi‐solid‐state potassium metal batteries (QSSKBs) coupled with two kinds of layered oxide cathodes demonstrate remarkable stability over 300 cycles, outperforming the liquid electrolyte counterparts. The QSSKB system provides a promising strategy for high‐efficiency, safe, and durable large‐scale energy storage.

Boosting K+-Ionic Conductivity of Layered Oxides via Regulating P2/P3 Heterogeneity and Reciprocity for Room-Temperature Quasi-Solid-State Potassium Metal Batteries.

Solid-state potassium metal batteries are promising candidates for grid-scale energy storage due to their low cost, high energy density and inherent safety. However, solid state K-ion conductors struggle with poor ionic conductivity due to the large ionic radius of K+-ions. Herein, we report precise regulation of phase heterogeneity and reciprocity of the P2/P3-symbiosis K0.62Mg0.54Sb0.46O2 solid electrolyte (SE) for boosting a high ionic conductivity of 1.6×10-4 S cm-1 at 25 °C. The bulk ionic conducting mechanism is explored by elucidating the effect of atomic stacking mode within the layered framework on K+-ion migration barriers. For ion diffusion at grain boundaries, the P2/P3 biphasic symbiosis property assists in tunning the SE microstructure, which crystallizes in rod-like particles with lengths of tens of micrometers facilitating long-distance ion transport and significantly decreasing grain boundary resistance. Potassium metal symmetric cells using the modified SE deliver excellent cycling life over 300 h at 0.1 mA cm-2 and a high critical current density of 0.68 mA cm-2. The quasi-solid-state potassium metal batteries (QSSKBs) coupled with two kinds of layered oxide cathodes demonstrate remarkable stability over 300 cycles, outperforming the liquid electrolyte counterparts. The QSSKB system provides a promising strategy for high-efficiency, safe, and durable large-scale energy storage.

Multifaceted insights into pentagonal BeP2 monolayer: From electrochemical to mechanical resilience for alkali-ion batteries using DFT

Herein, we elucidated the properties of a pentagonal BeP2 monolayer, emphasizing its robust dynamic, thermal, and mechanical stabilities, as well as its promising electrochemical characteristics. Combining density functional theory (DFT) with a thermodynamic energy decomposition scheme, we identified BeP2 as a potentially excellent 2D material for energy storage devices. It is characterized by large lattice parameters and semi-metallic behavior, exhibiting a zero density of states (DOS) at the Fermi level. It demonstrates favorable open-circuit voltages, low metal ion migration barriers, and negligible structural modifications for Na and K ions. The specific capacities of Li/Na/K reached remarkable values, surpassing those of most previously reported monolayers. Emerging ion battery technology necessitates solid, directly comparable data to establish an optimized standard organic solvent electrolyte. With this objective in mind, we systematically investigated systems combining two Li/Na/K salts with three different alkyl carbonate solvents. Furthermore, we proposed a defect in BeP2 to explore all possible avenues for sustaining the pentagonal BeP2 monolayer (supplementary Fig. S5 and S6). In summary, our findings strongly indicate that the pentagonal BeP2 monolayer holds considerable promise as an anode material for sodium-ion batteries (NIBs) and potassium-ion batteries (KIBs) owing to its high electrochemical and mechanical sustainability and excellent compatibility with electrolytes.

Recent Progress of Thin Crystal Engineering for Perovskite Solar Cells.

Metal halide perovskite single crystals hold promise for photovoltaics with high efficiency and stability due to their superior optoelectronic properties and weak bulk ion migration. The past several years have witnessed rapid development of single-crystal perovskite solar cells (PSCs) with efficiency rocketed from 6.5% to 24.3%, however, which still lags behind their polycrystalline counterparts. Moreover, the poor device stability under light illumination is contrary to the high ion migration barrier of perovskite single crystals. The key limiting factors should be the low crystalline quality and high surface defect density of solution-grown thin single crystals. Under this circumstance, a review paper summarizing the recent progress and challenges will be instructive for future development of this emerging field. In this manuscript, the crystal engineering used to enhance carrier transport and suppress carrier recombination in vertical single-crystal PSCs will be summarized initially, including crystal growth, component control, surface and interface modification. Subsequently, the application of perovskite single crystals in lateral single-crystal PSCs will be discussed and compared with the conventionally vertical structure. Finally, the challenges and proposed strategies for the development of single-crystal PSCs are provided.

Effects of Varying Nano-Montmorillonoid Content on the Epoxy Dielectric Conductivity

This study investigates the correlation between the interface structure and macroscopic dielectric properties of polymer-based nanocomposite materials. Utilizing bisphenol-A (BPA) epoxy resin (EP) as the polymer matrix and the commonly employed layered phyllosilicate montmorillonoid (MMT) as the nanometer-scale dispersive phase, nano-MMT/EP composites were synthesized using composite technology. The microstructure of the composite samples was characterized through XRD, FTIR, SEM, and TEM. Changes in the morphology of the nanocomposite interface were observed with varying MMT content, subsequently impacting dielectric polarization and loss. Experimental measurements of the dielectric spectrum of the nano-MMT/EP were conducted, and the influence of the material interface, at different nano-MMT contents, on the dielectric relaxation was analyzed. The study delves into the effect of the nanocomposite interface structure on ion dissociation and migration barriers, exploring the ionic conductivity of nano-MMT/EP. Lastly, an analysis of the impact of different nano-MMT contents on the dielectric conductivity is presented. From the experimental results, the arranging regularity of polymer molecules in the interface area raises. In the matrix, the ion migration barriers decrease significantly. The higher the MMT content in the interface, the lower the migration barrier is. Until the MMT content exceeds the threshold, the agglomerated micro-particles form, which decreases the polymers’ space distribution regularity, and the ions migration barrier raises. According to the changes in the rule of the ions migration barrier with the composite interface structure content, the reason for dielectric conductivity changes can be judged.

The C-BixSnSb composite toward fast-charging and long-life sodium-ion batteries

Sodium ion batteries (SIBs) fitted with high-rate and high-capacity anodes are attractive for their higher energy density and faster charging capability. However, it is still a challenge to develop high-energy SIBs with high power and long life, due to the sluggish kinetic and limited Na+ insertion in electrode materials. The inherent crystal structure and constituent element are two important factors to resolve the critical issues faced above. Taking the merits of layer-structure and middle-entropy, herein, we proposed and designed a high ion-conductive composite combing with ternary alloy and layered BixSnSb@C nanofibers, which eliminate ion migration barriers while maintaining the structural framework for superior rate property and cycle stability. Used as anode for SIBs, the multiphase BixSnSb@C with adjustable Bi content exhibits excellent Na storage capability as compared to their single phase counterpart. Specially, up to a rate of 132C (50 A g−1), the capacity is still as high as 400 mAh g−1, meanwhile, after 5000 charge and discharge cycles at a current density of 12C, the capacity still maintains 85 % of its initial capacity, which outperform the individual Bi- or SnSb-based materials. The superior electrochemical performances originate from the middle-entropy nature and layer structure of BiSnSb alloy, which can provide more channels for fast Na+ transport, and accommodate large volume changes. Besides, the activity energy and ions transport resistance of Na+ in different composites were evaluated. Furthermore, the full-cell coupled with NaNi1/3Fe1/3Mn1/3O2 as cathode was formed and a capacity retention of ∼80 % is realized in 100 cycles. The results show that the BixSnSb@C is a potential anode for fast-charging Na-ion batteries and could be used to guide the design of multi-component alloy-base anodes.

Exploring the potential of Mbenes in energy storage

MBene, a layered metal boride similar to MXene, has garnered significant attention in recent times. Nevertheless, there is still a lack of comprehensive understanding regarding their structure and properties, necessitating further research and investigation. In this study, theoretical calculations were employed first to study the binding energy, band structures and density of states of three MBenes, namely MoB, MgB2, and ZrB2, providing insights into their electronic characteristics. In addition, open circuit voltage (OCV) and adsorption energy were also conducted using the three MBenes as cathode materials for zinc ion batteries, indicating their low ion migration barrier and potential in energy storage application. Subsequently, MoB, MgB2, and ZrB2 were experimentally synthesized using etching or exfoliation method and utilized as cathode materials for zinc ion batteries. Results demonstrates that the specific capacity of MoB is 60 mAh g-1 at 0.1 A g-1. Systematic investigation including kinetics simulation and ex situ XRD suggests the cation insertion mechanism of the MoB electrodes. Building upon these findings, attempts were made to enhance the performance of MoB through the incorporation of 1 T-MoS2 composites, urea molecular intercalation. Notably, the modified composite exhibited a specific capacity exceeding 150 mAh g-1 at 0.1 A g-1, with a stable Coulombic efficiency of 100% after 100 cycles. This study provides novel directions and insights for the research of MBene in the context of aqueous zinc-ion batteries.

Superionic fluoride gate dielectrics with low diffusion barrier for two-dimensional electronics.

Exploration of new dielectrics with a large capacitive coupling is an essential topic in modern electronics when conventional dielectrics suffer from the leakage issue near the breakdown limit. Here, to address this looming challenge, we demonstrate that rare-earth metal fluorides with extremely low ion migration barriers can generally exhibit an excellent capacitive coupling over 20 μF cm-2 (with an equivalent oxide thickness of ~0.15 nm and a large effective dielectric constant near 30) and great compatibility with scalable device manufacturing processes. Such a static dielectric capability of superionic fluorides is exemplified by MoS2 transistors exhibiting high on/off current ratios over 108, ultralow subthreshold swing of 65 mV dec-1 and ultralow leakage current density of ~10-6 A cm-2. Therefore, the fluoride-gated logic inverters can achieve notably higher static voltage gain values (surpassing ~167) compared with a conventional dielectric. Furthermore, the application of fluoride gating enables the demonstration of NAND, NOR, AND and OR logic circuits with low static energy consumption. In particular, the superconductor-insulator transition at the clean-limit Bi2Sr2CaCu2O8+δ can also be realized through fluoride gating. Our findings highlight fluoride dielectrics as a pioneering platform for advanced electronic applications and for tailoring emergent electronic states in condensed matter.

Two-Terminal Perovskite Optoelectronic Synapse for Rapid Trained Neuromorphic Computation with High Accuracy.

Emerging neural morphological vision sensors inspired by biological systems that integrate image perception, memory, and information computing are expected to transform the landscape of machine vision and artificial intelligence. However, stable and reconfigurable light-induced synaptic behavior always relies on independent gateport modulation. Despite its potential, the limitations of uncontrollable defects and ionic characteristics have led to simpler, smaller, and more integration-friendly two-terminal devices being used as sidelines. In this work, the synergy between ion migration barriers and readout voltage is proven to be the key to realizing stable, reconfigurable, and precisely controllable postsynaptic current in two-terminal devices. Following the same mechanism, optical and electrical signal synchronous triggering is proposed to serve as a preprocessing method to achieve a recognition accuracy of 96.5%. Impressively, the gradual ion accumulation during the training process induces photocurrent evolution, serving as a reference for the dynamic learning rate and boosting accuracy to 97.8% in just 10 epochs. The PSC modulation potential under short optical pulse of 20 ns is also revealed. This optoelectronic device with perception, memory, and computation capabilities can promote the development of new devices for future photonic neural morphological circuits and artificial vision.

Strain Regulation of Mixed-Halide Perovskites Enables High-Performance Wide-Bandgap Photovoltaics.

Wide-bandgap mixed-halogen perovskite materials are widely used as top cells in tandem solar cells. However, serious open-circuit voltage (Voc ) loss restricts the power conversion efficiency (PCE) of wide-bandgap perovskite solar cells (PSCs). Herein, it is shown that the resulting methylammonium vacancies induce lattice distortion in methylammonium chloride-assisted perovskite film, resulting in an inhomogeneous halogen distribution and low Voc . Thus, a lattice strain regulation strategy is reported to fabricate high-performance wide-bandgap PSCs. Rubidium (Rb) cations are introduced to fill the A-site vacancy caused by the methylammonium volatilization, which alleviates shrinkage strain of the perovskite crystal. The reduced lattice distortion and increased halide ion migration barrier result in a homogeneous mixed-halide perovskite film. Due to improved carrier transport and suppressed nonradiative recombination, the Rb-treated wide-bandgap PSC (1.68eV) achieves an excellent PCE of 21.72%, accompanied by a high Voc of 1.22V. The resulting device maintains more than 90% of its initial PCE after 1500h under 1-sun illumination conditions.

Enhancing Sodium-Ion Transport by Hollow Nanotube Structure Design of a V5S8@C Anode for Sodium-Ion Batteries.

V5S8 has received extensive attention in the field of sodium-ion batteries (SIBs) due to its two-dimensional (2D) layered structure, and weak van der Waals forces between V-S accelerate the transport of sodium ions. However, the long-term cycling of V5S8 still suffers from volume expansion and low conductivity. Herein, a hollow nanotube V5S8@C (H-V5S8@C) with improved conductivity was synthesized by a solvothermal method to alleviate cracking caused by volume expansion. Benefiting from the large specific surface area of the hollow nanotube structure and uniform carbon coating, H-V5S8@C exhibits a more active site and enhanced conductivity. Meanwhile, the heterojunction formed by a few residual MoS2 and the outer layer of V5S8 stabilizes the structure and reduces the ion migration barrier with fast Na+ transport. Specifically, the H-V5S8@C anode provides an enhanced rate performance of 270.1 mAh g-1 at 15 A g-1 and high cycling stability of 291.7 mAh g-1 with a retention rate of 90.98% after 300 cycles at 5 A g-1. This work provides a feasible approach for the structural design of 2D layered materials, which can promote the practical application of fast-charging sodium-ion batteries.

First-principles study of slag impurity doped Na2Ti3O7 as anode material for Na-ion batteries

Na2Ti3O7 (NTO) has attracted significant attention as a promising anode material for sodium-ion batteries (SIBs). However, its practical electrochemical performance is hindered by its inherently low electronic conductivity. To address this limitation, researchers have turned to elemental doping as an effective strategy to enhance the conductivity of NTO electrodes. Interestingly, the process of purifying titanium for NTO synthesis often yields Al and Ca impurities, which can be harnessed as cost-effective dopants. In this study, we employ first-principles calculations to conduct a comprehensive investigation into the structural, electronic, and sodium ion diffusion properties of NTO when doped with Al and Ca, either individually or in combination. Doping system structure has good stability. Our findings reveal that both Al or Ca single-doping Our findings reveal that all the Al and Ca single-doping, and AlCa co-doping transform NTO from semiconducting into metallicity. Notably, the sodium ion migration barriers for Ca single-doping greatly decrease (0.13 eV) compared with that of pristine NTO (0.23 eV), indicating fast ion transport. The insights gained from our research hold promise for the development of cost-effective multi-component anode materials for SIBs.

Substitution of lead with tin suppresses ionic transport in halide perovskite optoelectronics.

Despite the rapid rise in the performance of a variety of perovskite optoelectronic devices with vertical charge transport, the effects of ion migration remain a common and longstanding Achilles' heel limiting the long-term operational stability of lead halide perovskite devices. However, there is still limited understanding of the impact of tin (Sn) substitution on the ion dynamics of lead (Pb) halide perovskites. Here, we employ scan-rate-dependent current-voltage measurements on Pb and mixed Pb-Sn perovskite solar cells to show that short circuit current losses at lower scan rates, which can be traced to the presence of mobile ions, are present in both kinds of perovskites. To understand the kinetics of ion migration, we carry out scan-rate-dependent hysteresis analyses and temperature-dependent impedance spectroscopy measurements, which demonstrate suppressed ion migration in Pb-Sn devices compared to their Pb-only analogues. By linking these experimental observations to first-principles calculations on mixed Pb-Sn perovskites, we reveal the key role played by Sn vacancies in increasing the iodide ion migration barrier due to local structural distortions. These results highlight the beneficial effect of Sn substitution in mitigating undesirable ion migration in halide perovskites, with potential implications for future device development.

Two-dimensional phosphorus carbides (β-PC) as highly efficient metal-free electrocatalysts for lithium-sulfur batteries: a first-principles study.

Li-S batteries are considered as the next-generation batteries due to their exceptional theoretical capacity. However, their practical application is hampered by the shuttling effects of lithium polysulfides (LiPSs) and the sluggish Li2S decomposition, particularly the slow conversion from Li2S2 to Li2S. Addressing these challenges, the quest for effective catalysts that can accelerate the conversion of LiPSs and enhance the performance of Li-S batteries is crucial. In this study, we explored the electrocatalytic activity of two-dimensional phosphorus carbides (β0-PC and β1-PC) in Li-S batteries based on first-principles calculations. Our findings reveal that these materials demonstrate optimal binding strengths (ranging from 1.09 to 1.83 eV) with long-chain LiPSs, effectively preventing them from dissolving into the electrolyte. Additionally, they show remarkable catalytic activity during the sulfur redox reaction (SRR), with ΔG being only 0.37 eV for β0-PC and 0.13 eV for β1-PC. The low energy barrier induced by β-PC enhances ion migration barrier and significantly expedites the charge/discharge cycles of Li-S batteries. Furthermore, we investigated the conversion dynamics of Li2S2 to Li2S, employing the computational lithium electrode (CLE) model. The excellent performance in these aspects underscores the potential of these materials as electrocatalysts for Li-S batteries, paving the way for advanced high-efficiency energy storage solutions.

Improved oxygen ion migration efficiency and resistive switching properties in SrFeOx memristor with vertical superlattice-like structure

The resistive switching (RS) behaviour between high and low resistance states in SrFeOx memristors originates from topological phase transition (TPT) induced by the migration of oxygen ions. Accelerating the migration of oxygen ions in the anisotropic crystal structure of SrFeO2.5 is of great importance for improving the RS properties and promoting the application for this TPT memristor. In this study, SrFeOx TPT memristors with different superlattice-like (SLL) structures were fabricated and the prepared devices with a vertical-type SIL structure display an ultra-low operation voltage of only 0.6 V, excellent cycling stability, data retention, and endurance performance. Moreover, the microstructures of vertical and horizontal SLL SrFeO2.5 were characterized with X-ray diffraction and transmission electron microscope. Furthermore, the differences in oxygen ion migration rate in the two structures were also tested by in-situ X-ray photoelectron spectroscopy. Finally, the optical band gaps and oxygen ion migration barriers of the two structures were calculated using first principles. All the characterizations and simulation results prove that the vertical type SrFeOx shows a higher oxygen ion migration efficiency. More encouragingly, the vertical SLL devices exhibit up to 96 % recognition accuracy for the Mixed National Institute of Standards and Technology image recognition task.

A topological nodal surface carbon honeycomb for sodium-ion battery anode

Motivated by the successful synthesis of three-dimensional (3D) graphene monoliths, we propose a 3D carbon honeycomb structure, tC40, composed of graphene-nanoribbons linked with 5-5-8 defects based on first-principles calculations. This structure is not only dynamically, thermally, and mechanically stable, but also possesses interesting electronic properties, including the multiple topological nodal surfaces on the high-symmetry plane k3=0 with double and quadruple degeneracies of bands in the reciprocal space, and the nontrivial surface states connecting different topological nodal surfaces parallel to the z-axis. By using the k·p model, we further show that, unlike previously reported nodal surfaces, the energy dispersion of the quadruply degenerated nodal surface is proportional to the k32, while the Hamiltonian of the doubly degenerated nodal surface is formed by the essential degeneracy of the valence and conduction bands. In addition, we explore the application of this nodal surface carbon as an anode material for sodium-ion batteries (SIBs), and find that tC40 exhibits good performance with a high reversible capacity of 186 mAh·g−1, a low sodium ion migration barrier of 0.1 eV, and a small charging/discharging volume change of 0.79 %. This work expands the family of topological carbon materials and their applications in SIBs.

Redox enhanced slow ion kinetics in oxide ceramics

AbstractThere is a growing interest in field‐assisted fast ceramic processing and long‐term service of electrochemical devices under harsh operation conditions. These extreme redox conditions can make some conventionally thought slow ions highly mobile in electrochemical materials and devices and greatly accelerate the microstructural evolution. Experimental observations for enhanced slow ion diffusion that controls mass transport include accelerated grain growth in zirconia and ceria under atmospheric and electrochemical reduction above 1000°C and lattice cavitation of high‐voltage Li‐rich layered cathodes of lithium‐ion batteries at room temperature. These observations cannot be explained by altered defect concentrations under defect chemistry arguments. Instead, they support hugely enhanced slow ion mobility. My colleagues and I recently proposed a new mechanism resulted from strong electron–phonon interactions and dynamic electronic relaxations at the saddle point of an ion hopping event, which significantly lowers the ion migration barrier. In this perspective article, the theory and its experimental and computational supports shall be discussed. Such an electronic effect holds even in nominally ionic ceramic materials with wide bandgaps and is expected to be general in many transition metal oxides. It rationalizes a variety of intriguing experimental observations and offers an electronic perspective on the redox enhancement of slow ion kinetics in structural, functional, and energy ceramics.

Dependence of lithium metal battery performances on inherent separator porous structure regulation

Boosting of rechargeable lithium metal batteries (LMBs) holds challenges because of lithium dendrites germination and high-reactive surface feature. Separators may experience structure-determined chemical deterioration and worsen Li plating-stripping behaviors when smoothly shifting from lithium-ion batteries (LIBs) to LMBs. This study precisely regulations the crystal structure of β-polypropylene and separator porous construction to investigate the intrinsic porous structure and mechanical properties determined electrochemical performances and cycling durability of LMBs. Crystal structure characterizations, porous structure analyses, and electrochemical cycling tests uncover appropriate annealing thermal stimulation concentrates β-lamellae thickness and enhances lamellae thermal stability by rearranging molecular chain in inferior β-lamellae, maximally homogenizing biaxial tensile deformation and resultant porous constructions. These even pores with high connectivity lower ion migration barriers, alleviate heterogeneous Li+ flux dispersion, stabilize reversible Li plating-stripping behaviors, and hinder coursing and branching of Li dendrites, endowing steady cell cycling durability, especially at higher currents due to the highlighted uncontrollable cumulation of dead Li, which offers new insights for the current pursuit of high-power density battery and fast charging technology. The suggested separator structure-chemical nature functions in ensuring cyclic cell stability and builds reliable relationships between separator structure design and practical LMBs applications.

In Situ Polymerizing Internal Encapsulation Strategy Enables Stable Perovskite Solar Cells toward Lead Leakage Suppression

AbstractDespite the outstanding power conversion efficiency (PCE) of perovskite solar cells (PSCs) achieved over the years, unsatisfactory stability and lead toxicity remain obstacles that limit their competitiveness and large‐scale practical deployment. In this study, in situ polymerizing internal encapsulation (IPIE) is developed as a holistic approach to overcome these challenges. The uniform polymer internal package layer constructed by thermally triggered cross‐linkable monomers not only solidifies the ionic perovskite crystalline by strong electron‐withdrawing/donating chemical sites, but also acts as a water penetration and ion migration barrier to prolong shelf life under harsh environments. The optimized MAPbI3 and FAPbI3 devices with IPIE treatment yield impressive efficiencies of 22.29% and 24.12%, respectively, accompanied by remarkably enhanced environmental and mechanical stabilities. In addition, toxic water‐soluble lead leakage is minimized by the synergetic effect of the physical encapsulation wall and chemical chelation conferred by the IPIE. Hence, this strategy provides a feasible route for preparing efficient, stable, and eco‐friendly PSCs.

Exploring Cathode Materials for Zn-Ion Batteries: A First-Principles Investigation

Aqueous zinc-ion batteries (ZIBs) are a promising technique for large-scale energy storage, however, the large ionic potential of Zn2+ ions leads to slow diffusion kinetics of Zn2+ ions in cathode hosts. To address this issue, we predicted two vanadium-based compounds for potential applications as cathode materials for ZIBs through the evolutionary algorithm. The dynamic, mechanical, and thermodynamic stabilities of the newly discovered ZnVO3 polymorphs were confirmed by ab initio calculations. CI-NEB results show impressively low Zn2+-ion migration barriers of 0.44 and 0.40 eV for the predicted P2/c and P21/c polymorphs, respectively. Furthermore, the P21/c-structured ZnVO3 exhibits a small band gap of 1.62 eV, a high voltage plateau of 1.16 V, and a trivial volume change upon charging, which may suggest excellent rate performance and a long cycle life when functioning as a cathode material for ZIBs. The work may provide fundamental guidance for the design and development of electrode materials featuring intrinsic fast Zn2+ ion transportation.