Increase In Unit Cell Volume Research Articles

Influence of calcination temperature on the 3D nanoscale topography of LaMnO3 thin films: A comprehensive surface analysis

In this paper, we present a comprehensive study on the 3D nanoscale topography of LaMnO3 thin films, focusing on the influence of calcination temperature on surface morphology. The study reveals significant structural, chemical, and morphological changes as a function of the calcination temperature. XRD analysis confirmed the formation of the orthorhombic LaMnO3 structure at 700 °C, 750 °C, and 800 °C, with increasing unit cell volume and crystallite size observed at higher temperatures. FTIR spectra identified characteristic functional groups associated with molecular vibrations, indicating the perovskite structure. SEM imaging showed grain growth with temperature, while EDS analysis confirmed compound formation and substrate interactions. AFM analysis revealed increased surface roughness with temperature, attributed to nucleation and crystal growth. Morphological and microtextural analyses further detailed changes in surface features, peaks, valleys, and voids. Fractal characterization highlighted variations in surface texture with temperature, with a decrease in dominant wavelength indicating changes in microtexture complexity. Overall, the findings provide insights into the temperature-dependent properties of LaMnO3 thin films, essential for optimizing growth conditions and understanding their potential applications in various fields.

Air‐stable Li3.12P0.94Bi0.06S3.91I0.18 solid‐state electrolyte with high ionic conductivity and lithium anode compatibility toward high‐performance all‐solid‐state lithium metal batteries

AbstractSulfide solid‐state electrolytes (SSEs) with superior ionic conductivity and processability are highly promising candidates for constructing all‐solid‐state lithium metal batteries (ASSLMBs). However, their practical applications are limited by their intrinsic air instability and serious interfacial incompatibility. Herein, a novel glass‐ceramic electrolyte Li3.12P0.94Bi0.06S3.91I0.18 was synthesized by co‐doping Li3PS4 with Bi and I for high‐performance ASSLMBs. Owing to the strong Bi‒S bonds that are thermodynamically stable to water, increased unit cell volume and Li+ concentration caused by P5+ substitution with Bi3+, and the in situ formed robust solid electrolyte interphase layer LiI at lithium surface, the as‐prepared Li3.12P0.94Bi0.06S3.91I0.18 SSE achieved excellent air stability with a H2S concentration of only 0.205 cm3 g−1 (after 300 min of air exposure), outperforming Li3PS4 (0.632 cm3 g−1) and the most reported sulfide SSEs, together with high ionic conductivity of 4.05 mS cm−1. Furthermore, the Li3.12P0.94Bi0.06S3.91I0.18 effectively improved lithium metal stability. With this SSE, an ultralong cyclability of 700 h at 0.1 mA cm−2 was realized in a lithium symmetrical cell. Moreover, the Li3.12P0.94Bi0.06S3.91I0.18‐based ASSLMBs with LiNi0.8Mn0.1Co0.1O2 cathode achieved ultrastable capacity retention rate of 95.8% after 300 cycles at 0.1 C. This work provides reliable strategy for designing advanced sulfide SSEs for commercial applications in ASSLMBs.

Improved cycle capability of Mn-doped Fe2TiO5 anode for lithium-ion batteries

Good cycling stability and high theoretical capacity are provided by Fe2TiO5 (iron titanate) as an electrode material due to its distinct crystal structure and numerous redox couples. The conventional ceramic method successfully and effectively synthesises the material. This study discloses the successful doping and replacement of Ti4+ with Mn4+ in the unit cell of Fe2TiO5 pseudobrookite, resulting in decreased band gap energy and a regular increase in unit cell volume with increased Mn-concentration. Doping improves the overall electrical conductivity due to a higher ratio of Ti3+ to Ti4+ which ultimately boosts the electrochemical performance as an anode in LIBs application. The Fe2Ti1-xMnxO5 (x = 0.2) achieves a high specific surface area of 338.6 m2 g−1 with an average pore size distribution of ∼10 nm, which is beneficial to reduce the Li-ion diffusion path and provides large contact areas between electrolyte and electrode surface. The Fe2Ti1-xMnxO5 (x = 0.2) stays ahead in its electrochemical performance compared to all counter partners delivering 765.6 mAh g−1 of initial discharge capacity and having a capacity retention of 392.3 mAh g−1 after 100 continuous charge discharge cycles at a current density of 100 mA g−1. Additionally, an excellent rate performance of 327.9 mAh g−1 is observed even at 5000 mA g−1. No further capacity fading is noted for another 45 cycles, demonstrating the structural stability of electrode material at variable current densities. The superior electrochemical results of Mn4+ doped Fe2TiO5 manifestly show the possibility of serving as an electrode material for high-performance battery applications.

Reversible Phase Transformations in a Double-Walled Diamondoid Coordination Network with a Stepped Isotherm for Methane.

Flexible metal-organic materials (FMOMs) with stepped isotherms can offer enhanced working capacity in storage applications such as adsorbed natural gas (ANG) storage. Unfortunately, whereas >1000 FMOMs are known, only a handful exhibit methane uptake of >150 cm3/cm3 at 65 atm and 298 K, conditions relevant to ANG. Here, we report a double-walled 2-fold interpenetrated diamondoid (dia) network, X-dia-6-Ni, [Ni2L4(μ-H2O)]n, comprising a new azo linker ligand, L- (L- = (E)-3-(pyridin-4-yldiazenyl)benzoate) and 8-connected dinuclear molecular building blocks. X-dia-6-Ni exhibited gas (CO2, N2, CH4) and liquid (C8 hydrocarbons)-induced reversible transformations between its activated narrow-pore β phase and γ, a large-pore phase with ca. 33% increase in unit cell volume. Single-crystal X-ray diffraction (SCXRD) studies of the as-synthesized phase α, β, and γ revealed that structural transformations were enabled by twisting of the azo moiety and/or deformation of the MBB. Further insight into these transformations was gained from variable temperature powder XRD and in situ variable pressure powder XRD. Low-temperature N2 and CO2 sorption revealed stepped Type F-II isotherms with saturation uptakes of 422 and 401 cm3/g, respectively. X-dia-6-Ni exhibited uptake of 200 cm3/cm3 (65 atm, 298 K) and a high CH4 working capacity of 166 cm3/cm3 (5-65 bar, 298 K, 33 cycles), the third highest value yet reported for an FMOM and the highest value for an FMOM with a Type F-II isotherm.

Impact of aliovalent La-doping on zinc oxide – A wurtzite piezoelectric

The development of high-performance low-cost electroactive films for energy conversion and electronic device applications is a key goal of current advanced materials and condensed matter physics research. Here, using solution-based scalable chemical spray pyrolysis, high-quality electroactive lanthanum-doped zinc oxide (i.e., Zn1-xLaxO) thin films are grown on silicon substrates, and the impact of aliovalent lanthanum doping is investigated using a suite of microstructural, optical and nanoscale scanning probe microscopy techniques. The synthesized polycrystalline thin films show hexagonal wurtzite crystal structure with an increased unit cell volume, crystallite size, and conductivity with lanthanum doping up to 4 at.% beyond which the thin films (6 at.%), however, exhibit a change in dominant crystalline orientation from (101) to (002) plane. Concurrently, at this optimal dopant concentration of 4–6 at.%, the electromechanical performance is enhanced by about 20 %, and polarity-dependent nanoscale electronic transport behaviour is revealed. Our study, therefore, provides key insights into the impact of the rare earth aliovalent lanthanum dopant on the electroactive and electronic properties of low-cost, functional thin films for sustainable energy and sensing applications.

Spin-disorder intervened avoidance of quantum criticality in B20 cubic Mn 1−xVx Si

The effect of negative chemical pressure with the substitution of transition metal V in an itinerant helimagnetically ordered MnSi, Mn 1−x V x Si with x = 0–0.1, is explored using dc and ac-susceptibilities. With increasing x, the manifestations are unaffected crystal structure with increasing unit cell volume, suppression of long-range magnetic order, weakening of itinerant character and reduced spin-cooperative phenomenon. The emergence of spin-glass behaviour for x⩾0.1 intervenes in the occurrence of quantum phase transition. The constructed concentration-temperature x-T phase diagram illustrates the substitution-driven changes in the magnetism of MnSi. Further, the study suggests that the presence of a precursor state can favour the formation of spin-textures in magnetically ordered compositions 0<x⩽0.05 below the ordering temperature.

Dynamic two-dimensional covalent organic frameworks.

Porous covalent organic frameworks (COFs) enable the realization of functional materials with molecular precision. Past research has typically focused on generating rigid frameworks where structural and optoelectronic properties are static. Here we report dynamic two-dimensional (2D) COFs that can open and close their pores upon uptake or removal of guests while retaining their crystalline long-range order. Constructing dynamic, yet crystalline and robust frameworks requires a well-controlled degree of flexibility. We have achieved this through a 'wine rack' design where rigid π-stacked columns of perylene diimides are interconnected by non-stacked, flexible bridges. The resulting COFs show stepwise phase transformations between their respective contracted-pore and open-pore conformations with up to 40% increase in unit-cell volume. This variable geometry provides a handle for introducing stimuli-responsive optoelectronic properties. We illustrate this by demonstrating switchable optical absorption and emission characteristics, which approximate 'null-aggregates' with monomer-like behaviour in the contracted COFs. This work provides a design strategy for dynamic 2D COFs that are potentially useful for realizing stimuli-responsive materials.

Building Nitridic Networks with Phosphorus and Germanium-from GeIIP2N4 to GeIVPN3.

Nitridophosphates and nitridogermanates attract high interest in current research due to their structural versatility. Herein, the elastic properties of GeP2N4 were investigated by single-crystal X-ray diffraction (XRD) upon compression to 44.4(1) GPa in a diamond anvil cell. Its isothermal bulk modulus was determined to be 82(6) GPa. At 44.4(1) GPa, laser heating resulted in the formation of multiple crystalline phases, one of which was identified as unprecedented germanium nitridophosphate GePN3. Its structure was elucidated from single-crystal XRD data (C2/c (no. 15), a = 8.666(5), b = 8.076(4), c = 4.691(2) Å, β = 101.00(7)°) and is built up from layers of GeN6 octahedra and PN4 tetrahedra. The GeN6 octahedra form double zigzag chains, while the PN4 tetrahedra are found in single zigzag chains. GePN3 can be recovered to ambient conditions with a unit cell volume increase of about 12%. It combines PV and GeIV in a condensed nitridic network for the first time.

The effect of Gd on the microstructure and electrochemical properties of Mg-Ni-based alloys

The Mg-Ni-based alloys have been extensively investigated as negative electrode materials in Nickel-Metal Hydride (Ni-MH) batteries. In this work, two Mg-Ni-based samples (Mg71Ni29 and Mg72.6Ni25.3Gd1.1) were prepared by means of melting. The X-ray diffraction (XRD), scanning electron microscope (SEM), galvanostatic charging/ discharging and other electrochemical measurements were used for the investigation. The results show that the Mg71Ni29 and Mg72.6Ni25.3Gd1.1 alloys include the characteristic peaks of Mg2Ni and the less strong characteristic peaks of Mg and MgNi2 phases. The diffraction peak of the major phase Mg2Ni of the Mg72.6Ni25.3Gd1.1 alloy is shifted to a small angle and its unit cell volume increases. With the addition of Gd, the alloy electrodes exhibits better cycling stability. After 50 charge/ discharge cycles, the capacity retention rate of the alloy electrode increase from 16% (Mg71Ni29) to 22% (Mg72.6Ni25.3Gd1.1). However, the maximum discharge capacity of the alloy electrode decrease from 134.3 mAh/g (Mg71Ni29) to 91.9 mAh/g (Mg72.6Ni25.3Gd1.1). The Mg72.6Ni25.3Gd1.1 alloy possess lower limiting current density IL and exhibit relatively high corrosion resistance against the alkaline solution. After Gd doping, the charge transfer capacity of the Mg72.6Ni25.3Gd1.1 alloy surface is increased.

The effects of hydrogen absorption in U3Si5 and its thermodynamic properties

The hydrogen absorption behavior of ▪ was examined using a Sieverts apparatus. Experimental results revealed the formation of a hydride phase with a stoichiometry reaching ▪ at pressures up to 250 kPa and temperatures below 300°C. By employing Van 't Hoff analysis, the enthalpy and entropy of formation for the newly formed hydride phase were measured as -19.73 kJ⋅mol−1 and -251.18 J⋅mol−1⋅T−1, respectively. Rietveld refinement showcased an expansion in lattice parameters a and c, resulting in an overall increase in unit cell volume of up to 8%; volume expansion can induce structural failures within the material.

Investigation of crystal structural and magnetic properties of titanium doped Pr0.67Ba0.33MnO3 perovskite manganites

Pr0.67Ba0.33Mn1-xTixO3 (x = 0 and 0.02) were synthesized using a conventional solid-state synthesis method to investigate the effect of Ti substitution on their magnetic and electrical transport properties. All the samples were structurally evaluated by XRD diffraction Rietveld refinement method which showed an increase in unit cell volume with increasing Ni content, indicating that Ti is partially substituted at Mn. Scanning electron microscopy (SEM) and energy dispersive X-tray (EDX) are used to examine the surface morphology and identified elements in the samples' compounds. Fourier transform infrared spectroscopy (FTIR) reveals that all the samples exhibit a transmission band in the range of 590 cm-1 - 610 cm-1 . For x = 0, magnetization measurements showed paramagnetic (PM) to ferromagnetic (FM) transition at the transition temperature, TC ∼ 213 K. For Ti-substituted samples, ferromagnetic (FM) to PM transition was reduced with Curie temperature (TC), decreasing from 213 K (x = 0) to 205 K (x = 0.02). On the other hand, the M(H) showed the presence of a linear graph for x = 0 and x = 0.02 which may be related to the presence of paramagnetic at room temperature.

Influence of iron substitution on structural, magnetic, and magnetocaloric properties of Tb2Fe17−xAlx compounds synthesized by arc melting

In the present work, the structure and magnetic and magnetocaloric properties of the Tb2Fe17−xAlx compounds with x=0,0.25,0.5,0.75, and 1 were studied. These compounds were synthesized by arc furnace without subsequent annealing. Their crystal structure is a Th2Ni17 hexagonal structure with a P63/mmc space group. The Rietveld refinement of the X-ray diffractograms allowed for determining the structural parameter variations with different amounts of aluminum. Lattice parameters and the unit cell volume increase with aluminum amounts while the c/a ratio remains nearly constant. The Tb2Fe17−xAlx compounds exhibit a second-order magnetic phase transition from a ferromagnetic state to a paramagnetic state. The Curie temperature (TC) increases with the aluminum content, the observed effect is due to the magnetovolumic effect. The saturation magnetization (MS) decreases with the increase of Al content. Magnetic entropy and relative cooling power (RCP) decrease as the aluminum content increases. Tb2Fe17−xAlx compounds have a moderate magnetocaloric effect and a tunable operating temperature interval.

Synthesis and optical properties of novel red-emitting phosphors Ba3Lu1–xEuxB9O18 (x = 0–0.85)

The novel red-emitting phosphors Ba3Lu1–xEuxB9O18 (x = 0, 0.1, 0.2, 0.3, 0.4, 0.5, 0.85) belonging to the Ba3REEB9O18 (REE – Y, Pr–Lu) family were successfully obtained by a multistep solid-phase synthesis. X-ray diffraction experiments revealed no phase transitions caused by the Eu3+ → Lu3+ isomorphic substitution in this series of solid solutions. An increase in the Eu3+ content leads to an expectable increase of hexagonal unit cell parameters and volume. Optical properties of the Ba3Lu1–xEuxB9O18 (x = 0–0.85) phosphors were investigated. The highest emission intensity was demonstrated by Ba3Lu0.6Eu0.4B9O18. The concentration quenching of luminescence was revealed for the x(Eu3+) > 0.4 samples. Concentration quenching, quantum yield and structural data were compared between three red-emitting Ba–Lu borates-phosphors (BLBO:Eu3+) containing independent crystallographic sites for the REE ions (n = 1–3) in crystal structure. It was revealed that the higher the number of nonequivalent cationic REE sites suitable for the Eu3+ → Lu3+ substitution, the higher the quantum yield taking into account practically equal amount of an optimal concentration of the activator-ion. Such an observation could be useful for a crystal chemical design of novel phosphors.

Long-Term Tests and Advanced Post-Test Characterizations of the Oxygen Electrode in Solid Oxide Electrolysis Cells

Solid Oxide cells (SOCs) are promising high-temperature electrochemical energy-conversion devices, which enable a fossil-free sustainable development. Nevertheless, performance degradation is still a bottleneck for the large-scale commercialization. The most commonly employed material for the air electrode is La1-xSrxCoy-1FeyO3-δ. The chemical decomposition of this material is known to considerably impact the cell performance [1,2].The studied cells are composed of a La0.6Sr0.4Co0.2Fe0.8O3 -δ (LSCF) current collecting layer (CCL) and a LSCF-Ce0.8Gd0.2O2 -δ (LSCF-GDC) composite for the air electrode, GDC for the barrier layer, (Y2O3)0.08(ZrO2)0.92 (YSZ) for the electrolyte and Ni-YSZ for the functional layer and the support layer of the fuel electrode. The present study aims to investigate the degradation occurring in the air electrode of a complete cell aged at 750°C for 2000 h in electrolysis mode. The cell degradation is assessed by electrochemical measurements, such as polarization curves and electrochemical impedance spectroscopy (EIS), and post-mortem characterizations of the air electrode using high resolution multimodal chemical imaging based on synchrotron X-ray diffraction (µ-XRD) in Paul Scherrer Institut (PSI, microXAS), complemented by X-ray photoelectron spectroscopy (XPS).The electrochemical characterizations performed at the beginning of the test and after ageing showed a decrease in the cell performance. Notably, a significant evolution at the high frequency region was observed in the impedance spectrum. However, the medium frequency region of the EIS, mainly ascribed to the air electrode using a physically-based multiscale model [3], did not show any particular evolution. Post-mortem characterizations using synchrotron µ-XRD technique showed an inter-diffusion layer (IDL) in between the GDC and YSZ layers, for both pristine and aged samples (Fig. 1). In addition, a slight increase in the LSCF unit cell volume was observed after ageing. Nevertheless, XPS results did not highlight any significant evolution in the Sr segregation after operation. According to the impedance spectra and the post-mortem analyses, the ageing of the air electrode seems to have a limited impact on the cell performance loss in these operating conditions.

A comparative study of structural, magnetic and catalytic properties of half doped nanocrystalline La0.5A0.5Mn0.5Fe0.5O3 (A = Ca, Sr) perovskite oxides: Highly efficient and versatile candidates for enhanced oxidative degradation of hazardous organic dyes at ambient conditions

This work presents a systematic study of half doped nanocrystalline La0.5A0.5Mn0.5Fe0.5O3 (A = Ca, Sr) perovskite oxides to examine the effect of A-site cation radius on structural, magnetic and catalytic properties via different characterization techniques. Rietveld refinements of powder X-ray diffraction data confirmed the orthorhombic symmetry for both the samples with Pbnm space group. The results show an increase in lattice parameters and unit cell volume with doping of larger A cation. The BET surface area for Ca and Sr-doped samples has been found to be 32.3 m2/g and 33.8 m2/g respectively. The magnetic properties of nano structured samples show magnetic inhomogeneity due to coexistence of ferromagnetic and antiferromagnetic interactions. The magnetization has enhanced in Sr-doped sample which may be associated with increase in double exchange interactions between mixed valence manganese ions through oxygen. Moreover, the synthesized nano samples have been employed to catalytic degradation of rhodamine B dye as model pollutant under normal atmospheric conditions and it has been found that Sr-doped sample has shown better catalytic dye degradation than Ca-doped (99% degradation in 25 min) due to the presence of greater number of Mn3+/Mn4+ redox couples as determined by iodometric titration. Additionally, methylene blue and methyl orange dyes were also tested for catalytic degradation by more active Sr-doped catalyst in order to check its versability.

Temperature-dependent dielectric measurements and structural properties of barium stannate (BaSnO3)

Cubic perovskite BaSnO3, synthesized by solid-state reaction method, was structurally characterized using temperature-dependent X-ray and Raman spectroscopy studies along with room temperature neutron diffraction analysis. Here, we report the effect of temperature on the structural parameters of BaSnO3 in correlation with dielectric properties. Sample homogeneity and elemental composition were studied by scanning electron microscopy and energy dispersive X-ray spectroscopy methods. The compound maintains cubic symmetry even at high temperatures and exhibits gradual increase in unit cell volume owing to thermal expansion. To understand high temperature phase transition, if any, and capacitance behavior, high temperature dielectric measurements were carried out. High value of dielectric constant was obtained at low frequencies as the temperature was increased, which may be due to the presence of oxygen vacancies or the lone-pair effect.

Structure and Electrical Conductivity of Bismuth- and Germanium-Doped Calcium Molybdates

Ca1 – 2xBi2xMo1 – xGexO4 solid solutions with a scheelite-like structure (space group I41/a) and the homogeneity range х = 0.0–0.4 were prepared using standard ceramic technology. The unit cell parameter с and unit cell volume increase as the dopant concentration increases due to the changing size of Ca/BiO8 polyhedra. The predominant thermal expansion of Ca/BiO8 polyhedra was inferred from the temperature-dependent unit cell parameters and Raman spectral patterns. The Ca/Bi–O and Mo/Ge–O bond lengths were calculated. The increasing dopant concentration decreases the thermal expansion coefficient of the ceramics and increases the electrical conductivity and activation energy of the complex oxides compared to the matrix compound. The effective oxygen diffusion coefficient is determined.

Vergasovaite to cupromolybdite topotactic transformation with crystal shape preservation

Abstract Thermal behavior of vergasovaite, ideally Cu3O(SO4)(MoO4), and its synthetic analog has been studied by high-temperature single-crystal X-ray diffraction in the temperature range of 300–1100 K. According to EMPA results, the empirical formulas are (Cu2.36Zn0.61)Σ2.97O[(Mo0.91S0.08V0.04)Σ1.03O4](SO4) for vergasovaite and Cu2.97O[(Mo0.92S0.09)Σ1.01O4](SO4) for its synthetic analog. The mineral is stable up to 950 ± 15 K; at 975 K, the unit-cell parameters and volume increase abruptly due to topotactic transformation of vergasovaite to cupromolybdite, Cu3O(MoO4)2. The transformation is accompanied by loss of sulfur (and excess copper) without destruction of the crystal. The thermal expansion of the vergasovaite structure is strongly anisotropic, being minimal along the [O2Cu6]8+ chains comprised of vertex-sharing OCu4 tetrahedra. This peculiar thermal behavior can be explained by the anisotropy of bond-length evolution in the Cu1O6 and Cu3O6 octahedra and the flexibility of the S-O-Cu and Mo-O-Cu bond angles. Synthetic Zn- and V-free analogs demonstrate negative thermal expansion at 425–625 K and melt at as low temperature as 700 K with no indication of transformation or recrystallization at least below 1200 K. The topotactic transformation observed in vergasovaite may have important implications for the design of novel materials and for understanding the alteration processes of copper minerals.

Isovalent substitution of vanadium in LiFePO4: Evolution of monoclinic α-Li3Fe2(PO4)3 phase

We report the synthesis and characterization of isovalent substitution of vanadium at phosphorus site in orthorhombic lithium iron phosphate (LiFePO4) nanoparticles by non-aqueous sol–gel method. Detailed analysis of X-ray diffraction patterns reveals the evolution of monoclinic α-Li3Fe2(PO4)3 phase and its formation is favored for the vanadium content higher than 20%. A continuous increase in unit cell volume of LiFePO4 is observed with increase in vanadium content from x = 0.05 to 0.20, followed by rapid decrease above x = 0.20, due to the creation of a greater number of Li-ion vacancies. FTIR studies demonstrate that the wavenumbers of various absorption maxima and the covalency strength parameter do not show a variation with x, thus confirm the substitution of vanadium in the form of VO4. Our results through Mössbauer and electron paramagnetic resonance spectroscopy unambiguously demonstrate the enhancement in the formation of α-Li3Fe2(PO4)3 phase for vanadium content higher than 20%.

First-Principles Study of the Effect of Ni-Doped on the Spinel-Type Mn-Based Cathode Discharge.

Spinel-type manganese oxide is considered as a typical cobalt-free high-voltage cathode material for lithium-ion battery applications because of its low cost, non-toxicity, and easy preparation. Nevertheless, severe capacity fading during charge and discharge limits its commercialization. Therefore, understanding the electrochemical properties and its modification mechanism of spinel-type manganese oxide for a lithium-ion battery is of great research interest. Herein, we presented a theoretical study regarding the discharge process of LiMn2O4 and LiNi0.5Mn1.5O4 using first-principles calculations based on density functional theory. We found that the discharge process is accompanied by an increase in unit cell volume and lattice distortion. Moreover, 25% Ni-substitution increases the average calculated voltage of LiMn2O4 from 3.83 to 4.61 V, which is very close to the experimental value. The electronic structure is further discussed to understand the mechanism of voltage increase. In addition, the Ni element also reduces the Li-ion diffusion barrier by 0.06 eV, which helps to improve the intrinsic rate performance of LiMn2O4. Our research can provide insight into how Ni-substitution influences the voltage and diffusion barrier of LiMn2O4 and pave the way for other spinel-type manganese oxide electrode applications.