Cathode Material For Batteries Research Articles

Improving the Performance of the Layered Nickel Manganese Oxide Cathode of Sodium-Ion Batteries by Direct Coating with Sodium Niobium Oxide.

This research highlights the efficacy of NaNbO3 as a coating for P2-Na2/3Ni1/3Mn2/3O2 cathodes in sodium-ion batteries. The coating enhances the kinetic behavior and cyclability of the electrochemical cells, as shown by electrochemical measurements. XRD analysis indicates that Nb does not incorporate into the cathode structure, implying a physical interaction between the coating and the cathode material. XRF analysis and EDX mapping confirm the actual composition and uniform dispersion of elements throughout the sample, while the electron micrographs evidence the occurrence of NaNbO3 particles modifying the surface of the layered oxide. The Ni4+/Ni3+ and Ni3+/Ni2+ redox pairs, along with the partially reversible oxidation of oxide to peroxide anions, contribute significantly to cell capacity, as revealed by XPS spectra. This last effect and the appearance of a co-intercalated phase at high voltage are positive factors to provide fast kinetics. Cyclic voltammograms show that samples coated with 2-3% NaNbO3 have superior rate capability, with high capacitive response and apparent diffusion coefficients. These samples also have low impedance at the electrode-electrolyte interface, which helps deliver a high capacity at 5C. Further cycling at 1C shows improved cyclability in the bare and 3% coated samples, due to their higher diffusion coefficients on charging. Notably, the 3% NaNbO3-coated sample exhibits excellent cyclability below 0 °C, making it a promising cathode material for sodium-ion batteries.

Electronic Confinement-Restrained Anti-Site Defects in Sodium-Rich Phosphates Toward Multi-Electron Transfer and High Energy Efficiency.

Sodium (Na) super-ionic conductor structured Na3MnTi(PO4)3 (NMTP) cathodes have garnered interest owing to their cost-effectiveness and high operating voltages. However, the voltage hysteresis phenomenon triggered by anti-site defects ( -ASD), namely, the occupation of Mn2+ in the Na2 vacancies in NMTP, leads to sluggish diffusion kinetics and low energy efficiency. This study employs an innovative electronic confinement-restrained strategy to achieve the regulation of -ASD. Partial replacement of titanium (Ti) with electron-rich vanadium (V) favors strong electronic interactions with Mn2+, restraining Mn2+ migration. The results suggest that this strategy can significantly increase the vacancy formation energy and migration energy barrier of manganese (Mn), thus inhibiting -ASD formation. As proof of this concept, an Na-rich Na3.5MnTi0.5V0.5(PO4)3 (NMTVP) material is designed, wherein the electronic interaction enhanced the redox activity and achieved more Na+ storage under high-voltage. The NMTVP cathode delivered a reversible specific capacity of up to 182.7 mAh g-1 and output an excellent specific energy of 513.8Wh kg-1, corresponding to ≈3.2 electron transfer processes, wherein the energy efficiency increased by 35.5% at 30C. Through the confinement effect of electron interactions, this strategy provides novel perspectives for the exploitation and breakthrough of high-energy-density cathode materials in Na-ion batteries.

Cracking Mechanism and Inhibition Strategies of Polycrystalline NCM Electrode Particles.

Developing a high-energy-density cathode material (LiNi1-x-yCoxMnyO2, NCM) for lithium-ion batteries is crucial to the electric vehicle and energy storage industries. However, the continuous insertion/extraction of Li+ generates diffusion-induced stress, causing NCM particles to crack or even pulverize, leading to battery capacity loss and limiting its wider commercial application. Current experimental studies are primarily postmortem examinations, and it is difficult to capture the particle cracking evolution. Simulation studies frequently ignore or simplify anisotropic volume contraction, demonstrating an insufficient understanding of the cracking mechanism of NCM polycrystalline particles, and cracking prevention strategies still need improvement. Therefore, we develop an anisotropic polycrystalline fracture phase-field model (AP-FPFM) that focuses on the anisotropic volume contraction of primary particles and precisely generates grain boundary distribution, coupling with Li+ diffusion, mechanical stress, and particle cracking. We employ AP-FPFM to demonstrate the behavior and mechanism of NCM polycrystalline particle cracking and illustrate the necessity and importance of anisotropic volume contraction to understand particle cracking. Furthermore, we explore the effects of average primary particle size, secondary particle size, and core-shell structure modulation on crack initiation and propagation and propose strategies to inhibit or migrate NCM polycrystalline particle cracking. This work provides theoretical support for revealing the cracking mechanism of anisotropic polycrystalline NCM particles and supplying optimization strategies to suppress particle cracking and improve the mechanical stability.

Boosting the synergistic activation of δ-MnO2 as cathode for aqueous zinc-ion batteries through Ni, Co co-doping

Layered δ-MnO2 is regarded as a promising cathode material for high-performance aqueous zinc-ion batteries (AZIBs) due to the sufficient interlayer spacing for the accommodation and migration of charge carriers. However, the sluggish activation process limits the reversible capacity, thus prevent their application. In this study, Ni-Co co-doped layered δ-MnO2 was designed to enhance ion diffusion capability and cycling stability. The influencing mechanism of Ni and Co on the long activation process are proposed by a comparative analysis between single doping and co-doping approaches. Specifically, the optimized co-doped δ-MnO2 maintained a high specific capacity of 200.2 mAh·g−1 with a capacity retention of 97.40 % after 700 cycles at 1 A·g−1. The co-doping approach exhibited a synergistic effect in suppressing Mn dissolution and enhancing ion diffusion capability. These findings provide new directions on boosting the synergistic activation process of manganese oxide and shed lights on the rational design of low-cost and high-safe batteries.

Modification study of Mg/W-doped LiNi0.9Mn0.1O2 layered oxide cathode materials for lithium-ion batteries

Modification study of Mg/W-doped LiNi0.9Mn0.1O2 layered oxide cathode materials for lithium-ion batteries

Stable electrochemical properties of trace titanium doping layered P3-type K0.5Mn0.92Ti0.08O2 cathode material for potassium ion batteries

The wide application of potassium ion batteries (PIBs) urgently requires the development of ideal cathode materials with low cost, good reaction kinetics and structural stability. Here, a titanium-doped K0.5Mn0.92Ti0.08O2 cathode material for potassium ion batteries is developed by doping modification strategy using a high-temperature solid-state method. The structure and performance structure-activity relationship of binary K0.5Mn1-xTixO2 cathode materials doped with non-electrochemically active element Ti4+ are studied experimentally and theoretically. With the introduction of Ti4+, when the doping amount is <10 mol%, the doped solid solution is hexagonal P3 phase, and the transition metal layer spacing increases. The non-equivalent doping affects the relative content of Mn3+/Mn4+, smoothes the redox peak in the electrochemical process, reduces the doping formation energy, and improves the structural stability. The ex-situ XRD fine structure study of the electrochemical process shows that the structural change of the material during the discharge process is suppressed after doping. The best Ti-doped cathode material K0.5Mn0.92Ti0.08O2 has an initial discharge capacity of 126.9 mAh·g−1 at a current density of 20 mA·g−1, and the capacity retention rate is 53.7 % after 100 cycles. This work provides a feasible strategy for the construction of stable electrode materials for PIBs.

Modified structure of vanadium oxide via cadmium doping and in-situ activation for high-performance aqueous zinc ion storage

Vanadium oxides are promising cathode materials for aqueous zinc-ion batteries, but they suffer from severe crystal collapse and poor electrical/ionic conductivity. Herein, we successfully synthesized the designed cadmium-doped, carbon-coated vanadium oxide precursor with abundant oxygen vacancies (Cd0.015V2O3-x@C) using a straightforward one-pot thermal reduction method, followed by in-situ activation to form a high-performance cathode material, Cd0.004V2O5-y·nH2O@C. We find that the interlayered water dramatically reduces the electrostatic force between zinc ions and V2O5-y layers, meanwhile, abundant oxygen vacancies and cadmium doping alter the material’s band structure, resulting in enhanced electronic and ionic conductivities. Leveraging these advantages, the phase transitioned Cd0.004V2O5-y·nH2O@C cathode delivers a remarkably high capacity of 420 mAh/g (0.2 A/g), an excellent rate capability of 198 mAh/g (20.0 A/g), and an outstanding capacity retention of 78.5 % after 3500 cycles (20 A/g). This synergistic structure modification strategy of elemental doping and in-situ activation offers a novel approach to design high-performance vanadium oxide-based cathodes for advanced aqueous batteries.

Enhancing the efficiency of two-electron zinc-manganese batteries enabled by Glycine complexation of manganese ions and compatibility with zinc anodes

Aqueous Zn//MnO2 batteries, leveraging the Mn2+/MnO2 conversion reaction, are gaining significant interest for their high redox potential and cost-effectiveness. However, they typically require a highly acidic environment to initiate this redox process. Herein, Glycine (Gly), a gentle and safe amino acid, is employed to enhance the effectiveness of depositing and dissolving Mn2+/MnO2. On one hand, Gly can complex with Mn2+, reducing its concentration and releasing H+. This not only promotes the dissolution of MnO2 but also increases the electrode potential. On the other hand, the Gly attaches to the Zn metal anode’s surface, shielding it from unwanted reactions. Hence, the assembled aqueous Zn//MnO2 battery exhibits an elevated output voltage during the discharge of 1.5 V with high coulombic efficiency (0.5 mAh cm−2 capacity), a long cycling life and excellent rate. This work showcases an efficient approach to enable the two-electron process of MnO2 cathode materials in aqueous zinc batteries.

Development of new cathode materials for all-iron redox flow batteries using hard carbon-based composites containing niobium pentoxide

We report in this study new cathodes for all-Fe RFBs synthesized using carbon flakes dispersed in plasticizing and hardening agents to obtain hard and dense carbon (HC) materials in the absence and presence (HC-Nb) of niobium pentoxide (Nb2O5). These cathode materials exhibited excellent resistance to wear in acidic solutions and larger potential intervals for water stability (e.g., 1200–1300 mV) compared to conventional graphite (e.g., 800 mV). These characteristics decreased the parasitic occurrence of hydrogen evolution reaction (HER) using a laboratory-made battery cell during the charging process. The latter was based on the Fe0/Fe2+ and Fe2+/Fe3+ redox couples present in the anode and cathode compartments, respectively. The different ex-situ and in-situ characterization studies evidenced that the presence of Nb2O5 in HCs substantially changed their physicochemical properties. The highest heterogenous kinetic rate constant (k0) representing the electrocatalytic activity for electron transfer was verified for the cathode containing 10 wt.% Nb2O5. An electromotive force (EMF) of 1.053 V was verified for the fully charged all-Fe RFB. Galvanostatic charge–discharge (GCD) studies revealed excellent coulombic efficiency (> 88 %) after 300 cycles. A pH control by acid addition as a function of the battery operation is necessary to avoid iron hydroxide formation on the anode’s surface.

Revealing the Role of Ruthenium on the Performance of P2-Type Na0.67Mn1-xRuxO2 Cathodes for Na-Ion Full-Cells.

Herein, P2-type layered manganese and ruthenium oxide is synthesized as an outstanding intercalation cathode material for high-energy density Na-ion batteries (NIBs). P2-type sodium deficient transition metal oxide structure, Na0.67Mn1-xRuxO2 cathodes where x varied between 0.05 and 0.5 are fabricated. The partially substituted main phase where x = 0.4 exhibits the best electrochemical performance with a discharge capacity of ≈170mAhg-1. The in situ X-ray Absorption Spectroscopy (XAS) and time-resolved X-ray Diffraction (TR-XRD) measurements are performed to elucidate the neighborhood of the local structure and lattice parameters during cycling. X-ray photoelectron spectroscopy (XPS) revealed the oxygen-rich structure when Ru is introduced. Density of States (DOS) calculations revealed the Fermi-Level bandgap increases when Ru is doped, which enhances the electronic conductivity of the cathode. Furthermore, magnetization calculations revealed the presence of stronger Ru─O bonds and the stabilizing effect of Ru-doping on MnO6 octahedra. The results of Time-of-flight secondary-ion mass spectroscopy (TOF-SIMS) revealed that the Ru-doped sample has more sodium and oxygenated-based species on the surface, while the inner layers mainly contain Ru-O and Mn-O species. The full cell study demonstrated the outstanding capacity retention where the cell maintained 70% of its initial capacity at 1C-rate after 500 cycles.

Fluorinated aggregated nanocarbon with high discharge voltage as cathode materials for alkali-metal primary batteries.

Due to its exceptionally high theoretical energy density, fluorinated carbon has been recognized as a strong contender for the cathode material in lithium primary batteries particularly valued in aerospace and related industries. However, CF x cathode with high F/C ratio, which enables higher energy density, often suffer from inadequate rate capability and are unable to satisfy escalating demand. Furthermore, their intrinsic low discharge voltage imposes constraints on their applicability. In this study, a novel and high F/C ratio fluorinated carbon nanomaterials (FNC) enriched with semi-ionic C-F bonds is synthesized at a lower fluorination temperature, using aggregated nanocarbon as the precursor. The increased presence semi-ionic C-F bonds of the FNC enhances conductivity, thereby ameliorating ohmic polarization effects during initial discharge. In addition, the spherical shape and aggregated configuration of FNC facilitate the diffusion of Li+ to abundant active sites through continuous paths. Consequently, the FNC exhibits high discharge voltage of 3.15V at 0.01C and superior rate capability in lithium primary batteries. At a high rate of 20C, power density of 33,694Wkg-1 and energy density of 1,250Wh kg-1 are achieved. Moreover, FNC also demonstrates notable electrochemical performance in sodium/potassium-CF x primary batteries. This new-type alkali-metal/CF x primary batteries exhibit outstanding rate capability, rendering them with vast potential in high-power applications.

Amorphous mesoporous sulfur-rich 1T/2H-MoS2 nanospheres as high-capacity cathode materials for advanced magnesium ion batteries

Two-dimensional layered-structure MoS2 has been explored as the promising cathode materials for magnesium ion batteries benefited by its wide layer distance and satisfactory capacity. However, such strong interaction between Mg2+ and MoS2 brings about the sluggish diffusion kinetics and irreversible electrochemical reaction, leading to a decreased specific capacity and poor rate capability. How to adopt its structure engineering and interface engineering to boost the Mg2+ diffusion kinetics and enhance the electrochemical reversibility of MoS2 is still a huge challenge. Herein, the amorphous sulfur-rich 1T/2H-MoS2 mesoporous nanospheres (a-MoS2+x, 0<x<1) have been developed via a facile one-pot hydrothermal route. Acted as a cathode material for magnesium ion batteries, owing to the cooperate effects of inherent rich active sites, high conductivity and wide layer distance induced by the coexistence of sulfur-rich, 1T phase and nearly amorphous features, the as-prepared a-MoS2+x demonstrates an ultra-high discharge capacity (438.7 mAh g−1 for 50 cycles at 0.1 A g−1), promising rate capability (97.6 mAh g−1 at 1.0 A g−1), and good cyclic stability (110 cycles at 0.5 A g−1), superior to the crystalline MoS2 (c-MoS2) and other previously reported MoS2 counterparts. Besides, the kinetics results indicate that the a-MoS2+x manifests good charge transfer and diffusion kinetics, and its entire charge storage is a combination of surface-controlled capacitance behavior and diffusion-controlled battery behavior. Moreover, some ex-situ Raman, XPS and HRTEM characterization techniques are employed to disclose the Mg2+ storage mechanism. Such remarkable magnesium storage properties of a-MoS2+x demonstrates its promising application as cathode for magnesium ion batteries.

Pre-inserting Mn2+/Zn2+ into NaV6O15 nanorods as high-stable and long lifespan cathodes for aqueous zinc-ion batteries

Vanadium-based compounds, characterized by diverse crystal structures, exhibit high theoretical capacities, and are regarded as potential cathode materials for aqueous zinc-ion batteries. Despite this, their development has been hindered by the sluggish diffusion of zinc ions and inadequate structural stability. In this study, we fabricated a stable monoclinic NaV6O15 nanorod via a simple hydrothermal synthesis. Mn2+ or Zn2+ ions are introduced into the crystal lattice to augment the interlayer spacing of NaV6O15, thereby enhancing the diffusion kinetics of Zn2+ ions. After pre-intercalating guest ions (Mn2+/Zn2+), the material experiences a morphological evolution from nanorods to nanobelts, which correlates with an expansion of the specific surface area and a proliferation of electrochemically active sites. This morphological alteration is associated with a marked enhancement in reversible capacity, reaching 278.1, 340.4, and 363.9 mAh/g for NVO, MNVO, and ZNVO, respectively, at 0.2 A/g. Furthermore, pre-intercalating guest ions not only expanded the interlayer spacing but also conferred structural robustness, leading to a pronounced enhancement in Zn2+ mobility and cyclability. Remarkably, the ZNVO cathode demonstrated a capacity retention of 118.4 % after 5000 cycles at a high current density of 5 A/g. Additionally, ex-situ XRD and XPS analyses elucidate that the Zn2+ storage in ZNVO is governed by the Zn2+ insertion/de-insertion mechanism. Our research offers a paradigm for the development of cathode materials for aqueous zinc-ion batteries.

Core-shell cobalt-iron@N-doped carbon: A high-performance cathode material for lithium-sulfur batteries.

Lithium-sulfur batteries hold great promise as energy storage systems, but the shuttle effect of lithium polysulfides (LiPS) and large volume variation limit their capacity and cycle life. We have developed CoFe alloy wrapped in N-doped porous carbon spheres (e-CF@NC) with a core-shell structure through simple copolymerization and pyrolysis. The nitrogen-doped porous carbon shell provides electron and ion transport channels and more active sites for electrolyte ion adsorption. The high chemically stable carbon can limit the segregation of polysulfides, further improving the battery cycling stability. Besides, the inside CoFe alloy particles catalyze the conversion between LiPS and Li2S, speeding up reaction kinetics and reducing solvation of active sites. Consequently, lithium-sulfur batteries with e-CF@NC-2 as the cathode display a high initial specific capacity of 1146 mA h g-1 at 0.1 C, excellent rate performance (891 mA h g-1 at 1 C, 741 mA h g-1 at 2 C), and satisfied cycle stability (average capacity decay rate of 0.033% per cycle at 1 C for 300 cycles), demonstrating significant application potential.

Linker length-dependent lithium storage of pyrene-4,5,9,10-tetraone-based conjugated organic polymer cathodes

Conjugated organic polymers (COPs) have been emerged as a class of cathode materials for lithium-ion batteries (LIBs) because of the rigid structural units and tunable properties. Nonetheless, their applications are still limited due to the poor conductivity and low cycling life. Herein, we design a series of pyrene-4,5,9,10-tetraone-based COPs (P(PTODB)-1, P(PTODB)-2, P(PTODB)-3), containing different number of benzene rings as linking units. Consequently, prolonging the linker lengths could effectively improve structural stability and extend π-conjugation, leading to the enhanced charge-storage capability. When tested as cathode materials for LIBs, the P(PTODB)-2 electrode delivers a better electrochemical performance with high capacity of 203 mA h g-1 after 100 cycles at 0.1 A g-1 (coulombic efficiency almost 100%) and excellent rate performance (150 mA h g-1 at 5 A g-1). In addition, the Li+ storage mechanism was carried out by ex situ Fourier transform infrared (FT-IR) and X-ray photoelectron spectroscopy (XPS) analysis. Eventually, our study brings forward the appropriately extended linker lengths to fabricate COP cathodes with high electrochemical properties.

Optimization of sodium-ion battery cathode performance by nickel-based Prussian blue epitaxial growth with iron-based Prussian blue core-shell structure

To address the structural defects and poor electrical conductivity of conventional Prussian blue analogues (PBAs) samples, in this study, nickel hexacyanoferrate (NiHCF) and nickel hexacyanoferrate epitaxially grown with iron hexacyanoferrate (Ni@FeHCF-X) series of samples were successfully synthesized by co-precipitation combined with epitaxial growth technique, and their structural and electrochemical properties were systematically characterized. X-ray powder diffractometer (XRD) results show that all the samples maintain a cubic crystal system structure, and the diffraction peaks of the (220) and (400) crystal planes are shifted to a lower angle with the epitaxial growth of ferric hexacyanoferrate (FeHCF). The successful embedding of Fe was confirmed by inductively coupled plasma (ICP) measurement data. Scanning electron microscope (SEM) images show that the samples are in a cubic morphology, and the surfaces gradually become rounded from sharp to rounded with the increase of the Fe content. High-resolution transmission electron microscope (HRTEM) and energy-dispersive spectrometer (EDS) analyses confirm the successful construction of the core-shell structure and the homogeneous distribution of the elements. Electrochemical testing showed that the Ni@FeHCF-X samples exhibited higher specific capacities and superior rate performance compared to NiHCF, particularly the Ni@FeHCF-4 sample, which delivered a high specific capacity of 73.4 mAh·g⁻¹ at a current density of 100 mA·g⁻¹, significantly outperforming the 38.2 mAh·g⁻¹ achieved by NiHCF. Additionally, the capacity retention rate of Ni@FeHCF-4 reached 42.16 %. Electrochemical impedance spectroscopy (EIS) further confirmed the reduced charge transfer resistance and enhanced reversibility of the electrochemical reactions in the Ni@FeHCF-X samples. These results demonstrate that Ni@FeHCF-4 significantly enhances the electrochemical performance of the samples in aqueous sodium-ion battery, providing new insights into the design of cathode materials for sodium-ion batteries.

Scalable production and performance optimization of Na3V2(PO4)3 cathode materials for sodium-ion batteries

The Na3V2(PO4)3 (NVP) cathode materials have garnered significant attention for grid energy storage due to their high theoretical capacity, rate performance, and cyclic stability. However, challenges persist, including inadequate electronic and ionic conductivity. This study addresses these issues through a novel solution-spray drying process using soluble precursors to achieve homogeneous mixing at the atomic level. This method not only promotes the formation of pure-phase NVP but also reduces carbon content effectively. Optimized heat treatment further enhances specific capacity, achieving 114 mAh/g at 0.1C with a coulombic efficiency of 99 %. These results highlight a scalable approach to improve the commercial viability of sodium-ion batteries by enabling efficient production of high-performance NVP cathode composites.

Promoting homogeneous tungsten doping in LiNiO2 through a grain boundary phase induced by excessive lithium

LiNiO2 (LNO) is one of the most promising cathode materials for lithium-ion batteries. Tungsten element in enhancing the stability of LNO has been researched extensively. However, the understanding of the specific doping process and existing form of W is still not perfect. This study proposes a lithium-induced grain boundary phase W doping mechanism. The results demonstrate that the introduced W atoms first react with the lithium source to generate a Li-W-O phase at the grain boundary of primary particles. With the increase of lithium ratio, W atoms gradually diffuse from the grain boundary phase to the interior layered structure to achieve W doping. The feasibility of grain boundary phase doping is verified by first principles calculation. Furthermore, it is found that the Li2WO4 grain boundary phase is an excellent lithium ion conductor, which can protect the cathode surface and improve the rate performance. The doped W can alleviate the harmful H2↔H3 phase transition, thereby inhibiting the generation of microcracks, and improving the electrochemical performance. Consequently, the 0.3wt% W-doped sample provides a significant improved capacity retention of 88.5% compared with the pristine LNO (80.7%) after 100 cycles at 2.8-4.3 V under 1 C.

Vertically stacked heterostructure in MoS2/rGO to accelerate ion diffusion kinetics for aqueous zinc ion batteries

The two-dimensional (2D) layered MoS2 is highly desirable as a host cathode material for aqueous zinc ion batteries (AZIBs) due to the typical lamellar structure bonded with weak van der Waals interlayer forces. Nevertheless, sluggish kinetics of Zn2+ diffusion in MoS2 usually leads to inferior Zn2+ storage capability. Herein, a vertically stacked heterostructure of reduced graphene oxide (rGO) and 1 T-2H phase mixed MoS2 (1 T-2H MoS2/rGO) is successfully realized through a bottom-up assembly method. The presence of graphene in the interlayer of MoS2 not only increases the interlayer spacing but also induces the phase transition of MoS2. The flower-like nanocomposite is featured with expanded interlayer spacing of 9.6 Å, abundant 1 T phase, and good hydrophilicity, which facilitate Zn2+ diffusion, charges transfer and electrolyte infiltration. Consequently, the 1 T-2H MoS2/rGO based AZIB achieves exceptional electrochemical performance: admirable specific capacity of 294.6 mAh g−1 at 0.2 A g−1, good rate capability (130.9 mAh g−1 at 4 A g−1), and excellent long-term stability (96.8 % capacity retention after 1600 cycles at 3 A g−1). Experimental and density functional theory (DFT) calculation results reveal that the vertical-stacked structure of MoS2/rGO accelerates Zn2+ diffusion kinetics and charges transfer by reducing the ions migrate energy barrier and band gap. The multiple ex situ characterizations demonstrate that the Zn2+ insertion/extraction process is accompanied by highly reversible phase transition between 2H and 1 T MoS2. This bottom-up assembly strategy can be extended to design more 2D materials with vertically stacked heterostructure as cathodes for high-performance AZIBs.

Exploring Electrolyte Adsorption on the Different Types of Layered Cathode Surfaces in Lithium-Ion Batteries via a Universal Neural Network Potential Method.

LiNi x Mn y Co z O2 (NCM) is a promising cathode material for lithium-ion batteries. Their long-term stability and impedance growth as cycles are strongly influenced by the properties of the cathode electrolyte interface (CEI), formed by the reaction between the electrolyte and electrode surface. Understanding of these interactions at the atomic level of the NCM electrode surface and electrolyte will provide a new strategic approach for the design of a highly functional CEI layer. In this study, we explored the influence of Ni content in transition metal layers on surface energies under different synthetic conditions and terminations using a density functional theory (DFT) validated universal neural network potential (UNNP) method. Furthermore, we investigated the adsorption of ethylene carbonate (EC) and dimethyl carbonate (DMC) on the most favorable NCM surfaces. EC and DMC displayed similar adsorption energy trends; however, differences were observed in the preferred configurations, which can affect the formation of the CEI.