In Situ TEM Observation of (Cr, Mn, Fe, Co, and Ni)3O4 High-Entropy Spinel Oxide Formation During Calcination at Atomic Scale.

High-entropy oxides (HEOs) are promising anode materials for lithium-ion batteries (LIBs), owing to their stable crystal structure, superionic conductivity, and high capacity. In this study, the (Cr, Mn, Fe, Co, and Ni)3O4 HEO via solid-state reaction is prepared. To improve the synthetic efficiency, it is necessary to understand the formation mechanism. Therefore, a high-resolution transmission electron microscopy (HRTEM) is used to record information during calcination at increasing temperature. The overall formation process included MnO2 and NiO aggregation at 500 °C, followed by (Mn, and Ni)3O4 combined with Co3O4 at 600 °C to form (Mn, Co, and Ni)3O4. At higher temperatures, Fe2O3 and Cr2O3 sequentially combined with (Mn, Co, and Ni)3O4 and formed the (Cr, Mn, Fe, Co, Ni)3O4 at 900 °C. In addition, the valence-state-changing mechanisms and ion arrangements of (Cr, Mn, Fe, Co, and Ni)3O4 are determined using electron energy loss spectroscopy (EELS) and extended X-ray absorption fine structure (EXAFS). This study successfully revealed the formation of HEO at atomic scale. The results provide valuable insights for improving the manufacturing process of (Cr, Mn, Fe, Co, and Ni)3O4 HEOs, which is expected to play a vital role in the development of anode materials for next-generation LIBs.

Tailored (La0.2Pr0.2Nd0.2Tb0.2Dy0.2)2Ce2O7 as a Highly Active and Stable Nanocatalyst for the Oxygen Evolution Reaction.

Designing highly active and robust catalysts for the oxygen evolution reaction is key to improving the overall efficiency of the water splitting reaction. It has been previously demonstrated that evaporation induced self-assembly (EISA) can be used to synthesize highly porous and high surface area cerate-based fluorite nanocatalysts, and that substitution of Ce with 50% rare earth (RE) cations significantly improves electrocatalyst activity. Herein, the defect structure of the best performing nanocatalyst in the series are further explored, Nd2Ce2O7, with a combination of neutron diffraction and neutron pair distribution function analysis. It is found that Nd3 + cation substitution for Ce in the CeO2 fluorite lattice introduces higher levels of oxygen Frenkel defects and induces a partially reduced RE1.5Ce1.5O5 + x phase with oxygen vacancy ordering. Significantly, it is demonstrated that the concentration of oxygen Frenkel defects and improved electrocatalytic activity can be further enhanced by increasing the compositional complexity (number of RE cations involved) in the substitution. The resulting novel compositionally-complex fluorite- (La0.2Pr0.2Nd0.2Tb0.2Dy0.2)2Ce2O7 is shown to display a low OER overpotential of 210 mV at a current density of 10 mAcm-2 in 1M KOH, and excellent cycling stability. It is suggested that increasing the compositional complexity of fluorite nanocatalysts expands the ability to tailor catalyst design.

Challenges and Strategies for Synthesizing High Performance Micro and Nanoscale High Entropy Oxide Materials.

High-entropy oxide micro/nano materials (HEO MNMs) have shown broad application prospects and have become hot materials in recent years. This review comprehensively provides an overview of the latest developments and covers key aspects of HEO MNMs, by discussing design principles, computer-aided structural design, synthesis challenges and strategies, as well as application areas. The analysis of the synthesis process includes the role of high-throughput process in large-scale synthesis of HEOs MNMs, along with the effects of temperature elevation and undercooling on the formation of HEO MNMs. Additionally, the article summarizes the application of high-precision and in situ characterization devices in the field of HEO MNMs, offering robust support for related research. Finally, a brief introduction to the main applications of HEO MNMs is provided, emphasizing their key performances. This review offers valuable guidance for future research on HEO MNMs, outlining critical issues and challenges in the current field.

Nanoflower-Like High-Entropy Co-Fe-Cr-Mo-Mn Spinel for Oxygen Evolution.

Oxygen evolution reaction (OER) is the key anode reaction of electrolytic water. To improve the slow OER kinetics, we synthesize nanoflower-like Co-Fe-Cr-Mo-Mn high-entropy spinel (HES) nanosheets on nickel foam (NF) by one-step solvothermal method, which exhibit an overpotential (η10) of only 188 mV at 10 mA cm-2, much lower than bimetallic CoFeOx/NF (233 mV), trimetallic CoFeCrOx/NF (211 mV), and tetrametallic CoFeCrMoOx/NF (200 mV). The OER overpotential decreases with the increase of the number of metals, indicating that the formation of HES has a positive effect on the improvement of electrocatalytic performance, since the synergistic effect between different metals enhances the charge transfer rate and decreases reaction barrier. In-situ Raman spectra demonstrate that the formation of γ-NiOOH on the HES surface is a crucial active species for the OER. This work demonstrates a simple and efficient synthesis method to prepare nanoflower-like high-entropy electrocatalysts for efficient OER electrocatalysis.

Boosting N2O Catalytic Decomposition by the Synergistic Effect of Multiple Elements in Cobalt-Based High-Entropy Oxides.

Nitrous oxide (N2O) has a detrimental impact on the greenhouse effect, and its efficient catalytic decomposition at low temperatures remains challenging. Herein, the cobalt-based high-entropy oxide with a spinel-type structure (Co-HEO) is successfully fabricated via a facile coprecipitation method for N2O catalytic decomposition. The obtained Co-HEO catalyst displays more remarkable catalytic performance and higher thermal stability compared with single and binary Co-based oxides, as the temperature of 90% N2O decomposition (T90) is 356 °C. A series of characterization results reveal that the synergistic effect of multiple elements enhances the reducibility and augments oxygen vacancy in the high-entropy system, thus boosting the activity of the Co-HEO catalyst. Moreover, density functional theory (DFT) calculations and the temperature-programmed surface reaction (TPSR) with isotope labeling demonstrate that N2O decomposition on the Co-HEO catalyst follows the Langmuir-Hinshelwood (L-H) mechanism with the promotion of abundant oxygen vacancies. This work provides a fundamental understanding of the synergistic catalytic effect in N2O decomposition and paves the way for the novel environmental catalytic applications of HEO.

Rapid Joule-Heating Synthesis for Manufacturing High-Entropy Oxides as Efficient Electrocatalysts.

High-entropy oxide (HEO) including multiple principal elements possesses great potential for various fields such as basic physics, mechanical properties, energy storage, and catalysis. However, the synthesis method of high-entropy compounds through the traditional heating approach is not conducive to the rapid properties screening, and the current elemental combinations of HEO are also highly limited. Herein, we report a rapid synthesis method for HEO through the Joule-heating of nickel foil with dozens of seconds. High-entropy rocksalt oxides (HERSO) with the new elemental combination, high-entropy spinel oxides (HESO), and high-entropy perovskite oxide (HEPO) have been synthesized through the Joule-heating. The synthesized HERSO with new elemental combinations proves to be a great promotion of OER activity due to the synergy of multiple components and the continuous electronic structure experimentally and theoretically. The demonstrated synthesis approach and the new component combination of HERSO provide a broad platform for the development of high-entropy materials and catalysts.

Rapid Synthesis of High-Entropy Oxide Microparticles.

High-entropy nanoparticles have received notable attention due to their tunable properties and broad material space. However, these nanoparticles are not suitable for certain applications (e.g., battery electrodes), where their microparticle (submicron to micron) counterparts are more preferred. Conventional methods used for synthesizing high-entropy nanoparticles often involve various ultrafast shock processes. To increase the size thereby achieving high-entropy microparticles, longer reaction time (e.g., heating duration) is usually used, which may also lead to undesired particle overgrowth or even densified microstructures. In this work, an approach based on Joule heating for synthesizing high-entropy oxide (HEO) microparticles with uniform elemental distribution is reported. In particular, two key synthesis conditions are identified to achieve high-quality HEO microparticles: 1) the precursors need to be loosely packed to avoid densification; 2) the heating time needs to be accurately controlled to tens of seconds instead of using milliseconds (thermal shock) that leads to nanoparticles or longer heating duration that forms bulk structures. The utility of the synthesized HEO microparticles for a range of applications, including high-performance Li-ion battery anode and water oxidation catalyst. This study opens up a new door toward synthesizing high-entropy microparticles with high quality and broad material space.

Holey Lamellar High-Entropy Oxide as an Ultra-High-Activity Heterogeneous Catalyst for Solvent-free Aerobic Oxidation of Benzyl Alcohol.

The development of noble-metal-free heterogeneous catalysts is promising for selective oxidation of aromatic alcohols; however, the relatively low conversion of non-noble metal catalysts under solvent-free atmospheric conditions hinders their industrial application. Now, a holey lamellar high entropy oxide (HEO) Co0.2 Ni0.2 Cu0.2 Mg0.2 Zn0.2 O material with mesoporous structure is prepared by an anchoring and merging process. The HEO has ultra-high catalytic activity for the solvent-free aerobic oxidation of benzyl alcohol. Up to 98 % conversion can be achieved in only 2 h, to our knowledge, the highest conversion of benzyl alcohol by oxidation to date. By regulating the catalytic reaction parameters, benzoic acid or benzaldehyde can be selectively optimized as the main product. Analytical characterizations and calculations provide a deeper insight into the catalysis mechanism, revealing abundant oxygen vacancies and holey lamellar framework contribute to the ultra-high catalytic activity.

Hollow-Structured and Polyhedron-Shaped High Entropy Oxide toward Highly Active and Robust Oxygen Evolution Reaction in a Full pH Range.

High entropy metal oxides (HEO) are superior to many reactions involving multi-step elementary reactions. However, controlled synthesis of hollow-structured HEO catalysts, which offers large surface area and fast mass transfer kinetics, remains challenging and unexplored due to the complicated metal precursors. Herein, a metal organic framework-templated synthesis of hollow-structured and polyhedron-shaped HEO catalysts assembled with ultra-small nanoparticles, with up to ten metal elements, can be achieved, by taking advantage of the ion-exchange method. ZnFeNiCuCoRu-O HEO catalyst displays excellent activity and ultra-stability for oxygen evolution reaction in full pH range, with an overpotential of 170 mV at a current density of 10 mA cm-2 , a Tafel slope of 56 mV dec-1 , and a decay of activity by 7% in 30 h in alkaline medium, as well as a 12% and 8% decay in acidic and neutral medium, respectively. DFT calculation indicates that the energy barrier of the potential determining step on Ru-Fe bridge site is significantly lower than any other Ru-related bridge sites for the unique hollow structured HEO structures. This work highlights the importance of ion-exchange method in preparing highly stable and active hollow-structured HEOs catalysts toward highly efficient energy conversion and storage devices.

Porous High-Entropy Oxide Anode Materials for Li-Ion Batteries: Preparation, Characterization, and Applications.

High-entropy oxides (HEOs), as a new type of single-phase solid solution with a multi-component design, have shown great potential when they are used as anodes in lithium-ion batteries due to four kinds of effects (thermodynamic high-entropy effect, the structural lattice distortion effect, the kinetic slow diffusion effect, and the electrochemical "cocktail effect"), leading to excellent cycling stability. Although the number of articles on the study of HEO materials has increased significantly, the latest research progress in porous HEO materials in the lithium-ion battery field has not been systematically summarized. This review outlines the progress made in recent years in the design, synthesis, and characterization of porous HEOs and focuses on phase transitions during the cycling process, the role of individual elements, and the lithium storage mechanisms disclosed through some advanced characterization techniques. Finally, the future outlook of HEOs in the energy storage field is presented, providing some guidance for researchers to further improve the design of porous HEOs.

General Synthesis of High-Entropy Oxide Nanofibers.

The discovery of high-entropy oxides (HEOs) in 2015 has provided a family of potential solid catalysts, due to their tunable components, abundant defects or lattice distorts, excellent thermal stability (ΔG↓ = ΔH - TΔS↑), and so on. When facing the heterogeneous catalysis by HEOs, the micrometer bulky morphology and low surface areas (e.g., <10 m2 g-1) by traditional synthesis methods obstructed their way. In this work, an electrospinning method to fabricate HEO nanofibers with diameters of 50-100 nm was demonstrated. The key point lay in the formation of one-dimensional filamentous precursors, during which the uniform dispersion of five metal species with disordered configuration would help to crystallize into single-phase HEOs at lower temperatures: inverse spinel (Cr0.2Mn0.2Co0.2Ni0.2Fe0.2)3O4 (400 °C), perovskite La(Mn0.2Cu0.2Co0.2Ni0.2Fe0.2)O3 (500 °C), spinel Ni0.2Mg0.2Cu0.2Mn0.2Co0.2)Al2O4 (550 °C), and cubic Ni0.2Mg0.2Cu0.2Zn0.2Co0.2O (750 °C). As a proof-of-concept, (Ni3MoCoZn)Al12O24 nanofiber exhibited good activity (CH4 Conv. > 96%, CO2 Conv. > 99%, H2/CO ≈ 0.98), long-time stability (>100 h) for the dry reforming of methane (DRM) at 700 °C without coke deposition, better than control samples (Ni3MoCoZn)Al12O24-Coprecipitation-700 (CH4 Conv. < 3%, CO2 Conv. < 7%). The reaction mechanism of DRM was studied by in situ infrared spectroscopy, CO2-TPD, and CO2/CH4-TPSR. This electrospinning method provides a synthetic route for HEO nanofibers for target applications.

Intergrating Hollow Multishelled Structure and High Entropy Engineering toward Enhanced Mechano-Electrochemical Properties in Lithium Battery.

Hollow multishelled structures (HoMSs) are attracting great interest in lithium-ion batteries as the conversion anodes, owing to their superior buffering effect and mechanical stability. Given the synthetic challenges, especially elemental diffusion barrier in the multimetal combinations, this complex structure design has been realized in low- and medium-entropy compounds so far. It means that poor reaction reversibility and low intrinsic conductivity remain largely unresolved. Here, a hollow multishelled (LiFeZnNiCoMn)3O4 high entropy oxide (HEO) is developed through integrating molecule and microstructure engineering. As expected, the HoMS design exhibits significant targeting functionality, yielding satisfactory structure and cycling stability. Meanwhile, the abundant oxygen defects and optimized electronic structure of HEO accelerate the lithiation kinetics, while the retention of the parent lattice matrix enables reversible lithium storage, which is validated by rigorous in situ tests and theoretical simulations. Benefiting from these combined properties, such hollow multishelled HEO anode can deliver a specific capacity of 967 mAh g-1 (89% capacity retention) after 500 cycles at 0.5 A g-1. The synergistic lattice and volume stability showcased in this work holds great promise in guiding the material innovations for the next-generation energy storage devices.

Low-Temperature Synthesis of Mesoporous Half-Metallic High-Entropy Spinel Oxide Nanofibers for Photocatalytic CO2 Reduction.

High-entropy oxides (HEOs) exhibit great prospects owing to their varied composition, chemical adaptability, adjustable light-absorption ability, and strong stability. In this study, we report a strategy to synthesize a series of porous high-entropy spinel oxide (HESO) nanofibers (NFs) at a low temperature of 400 °C by a sol-gel electrospinning technique. The key lies in selecting six acetylacetonate salt precursors with similar coordination abilities, maintaining a high-entropy disordered state during the transformation from stable sols to gel NFs. The as-synthesized HESO NFs of (NiCuMnCoZnFe)3O4 show a high specific surface area of 66.48 m2/g, a diverse elemental composition, a dual bandgap, half-metallicity property, and abundant defects. The diverse elements provide various synergistic catalytic sites, and oxygen vacancies act as active sites for electron-hole separation, while the half-metallicity and dual-bandgap structure offer excellent light absorption ability, thus expanding its applicability to a wide range of photocatalytic processes. As a result, the HESO NFs can efficiently convert CO2 into CH4 and CO with high yields of 8.03 and 15.89 µmol g-1 h-1, respectively, without using photosensitizers or sacrificial agents.

Role of oxygen vacancy in spinel (FeCoNiCrMn)3O4 high entropy oxides prepared via two different methods for the selective CH bond oxidation of p-chlorotoluene.

The selective CH bond oxidation of aromatic hydrocarbon is an interesting but challenging task, it is desirable to develop efficient heterogeneous non-noble metal catalyst for this reaction. Herein, two kinds of spinel (FeCoNiCrMn)3O4 high entropy oxides were fabricated via two different methods (i.e., c-FeCoNiCrMn, prepared by a co-precipitation method, and m-FeCoNiCrMn, prepared by physically mixing method). Different from traditional environmentally-unfriendly Co/Mn/Br system, the prepared catalysts were employed for the selective CH bond oxidation of p-chlorotoluene to p-chlorobenzaldehyde in a green approach. Compared to m-FeCoNiCrMn, c-FeCoNiCrMn have smaller particles size and larger specific surface area, which were related to the enhanced catalytic activity. More importantly, characterization results disclosed that abundant oxygen vacancies were formed over c-FeCoNiCrMn. Such a result facilitated the adsorption of p-chlorotoluene on the catalyst surface and promoted the formation of *ClPhCH2O intermediate as well as the desired p-chlorobenzaldehyde, as revealed by DFT (Density functional theory) calculations. Besides, scavenger tests and EPR (Electron paramagnetic resonance) results indicated that hydroxyl radical derived from H2O2 homolysis was the main active oxidative species for this reaction. This work revealed the role of oxygen vacancy in spinel high entropy oxide and also demonstrated its promising application for the selective CH bond oxidation in an environmentally-benign approach.

Flexoelectric Catalysts Based on Hierarchical Wrinkling Surface of Centrosymmetric High-Entropy Oxide.

A high-entropy oxide nanocomposite with Ag(CuZn)(AlCr)2O4 and CuO phases is fabricated to form an abundantly hierarchical wrinkled surface. Application of a mechanical force to the nanocomposite resulted in a nonhomogeneous strain gradient at the interface between the Ag(CuZn)(AlCr)2O4 and CuO phases, changing the local charge distribution and creating flexoelectric polarization that delayed electron/hole recombination. Transmission electron microscopy energy-dispersive X-ray spectroscopy mapping revealed that the Ag, Cu, Zn, Al, Cr, and O elements were highly distributed throughout the nanocomposite. The nanocomposite produced 2116 µmol·g-1 h-1 of H2 without external light irradiation, which is 980% higher than the H2 produced by the same nanocomposite under the photocatalytic process. A strong electrical field is observed at the interface between the Ag(CuZn)(AlCr)2O4 and CuO phases, demonstrating that a flexoelectric potential (flexopotential) is established at the structural boundaries because the strain gradient is localized at these interfaces. The nanocomposite is a promising approach for environmentally friendly energy production.

Microwave solvothermal synthesis of Component-Tunable High-Entropy oxides as High-Efficient and stable electrocatalysts for oxygen evolution reaction.

Transition-metal-based high-entropy oxides (HEOs) are appealing electrocatalysts for oxygen evolution reaction (OER) due to their unique structure, variable composition and electronic structure, outstanding electrocatalytic activity and stability. Herein, we propose a scalable high-efficiency microwave solvothermal strategy to fabricate HEO nano-catalysts with five earth-abundant metal elements (Fe, Co, Ni, Cr, and Mn) and tailor the component ratio to enhance the catalytic performance. (FeCoNi2CrMn)3O4 with a double Ni content exhibits the best electrocatalytic performance for OER, namely low overpotential (260 mV@10 mA cm-2), small Tafel slope and superb long-term durability without obvious potential change after 95 h in 1 M KOH. The extraordinary performance of (FeCoNi2CrMn)3O4 can be attributed to the large active surface area profiting from the nano structure, the optimized surface electronic state with high conductivity and suitable adsorption to intermediate benefitting from ingenious multiple-element synergistic effects, and the inherent structural stability of the high-entropy system. In addition, the obvious pH value dependable character and TMA+ inhibition phenomenon reveal that the lattice oxygen mediated mechanism (LOM) work together with adsorbate evolution mechanism (AEM) in the catalytic process of OER with the HEO catalyst. This strategy provides a new approach for the rapid synthesis of high-entropy oxide and inspires more rational designs of high-efficient electrocatalysts.

Toluene catalytic oxidation over gold catalysts supported on cerium-based high-entropy oxides.

A series of cerium-based high-entropy oxide catalysts (the ratio of CeO2 and HEO is 1:1) was prepared by a solid-state reaction method, which exploit their unique structural and performance advantages. The Ce-HEO-T samples can achieve 100% toluene conversion rate above 328°C when they were used as catalysts directly. Subsequently, the Ce-HEO-500 exhibited the lowest temperature for toluene oxidation was used as a support to deposit different amounts of Au for a further performance improvement. Among all of prepared samples, Au/Ce-HEO-500 with a moderate content of Au (0.5 wt%) exhibited the lowest temperature for complete combustion of toluene (260°C), which decreased nearly 70°C compared with Ce-HEO-500 support. Moreover, it also showed excellent stability for 60 h with 98% toluene conversion rate. Most importantly, under the condition of 5 vol.% H2O vapour, the toluene conversion rate remained unchanged and even increased slightly compared with that in dry air, exhibiting excellent water resistance. Combined with the characterizations of XRD, SEM, TEM, BET, Raman, H2-TPR and XPS, it was found that the high dispersion of active Au NPs, the special high-entropy structure and the synergistic effect between Au and Ce, Co, Cu are the key factors when improving the catalytic performance in the Au/Ce-HEO-500 catalyst.

Efficient removal of tetracycline hydrochloride by high entropy oxides in visible photo-Fenton catalytic process.

A novel type of oxide material, high entropy oxide (Mn0.2Fe0.2Co0.2Ni0.2Cu0.2)3O4 (MFO) composites with spinel structure were successfully synthesized by a simple solution combustion in this paper, and it was first applied to the degradation of antibiotic organic pollutants in water by photo-Fenton. SEM and BET characterization showed that the composite was porous and had a large specific surface area. XPS results showed that Fe, Mn, Cu, Co and Ni all participated in the redox reaction of the catalytic process. The redox pairs of Mn2+/Mn3+, Cu+/Cu2+, Co2+/Co3+, Ni2+/Ni3+ can accelerate the Fe2+/Fe3+ redox cycling in MFO to activate H2O2 and produce more reactive oxygen species. The catalytic performance of MFO composite was investigated using tetracycline hydrochloride (TC-HCl) as a model pollutant. The results displayed that the degradation rate of TC-HCl by MFO was 92.9% when the initial pH was 4, the dose of H2O2 was 50 mM, and the irradiation time was 60 min. The high entropy oxide MFO composites could build up an internal electric field, which restrains electron-hole recombination, improves the transfer of photogenerated charge carriers and maximize photocatalytic property. In addition, the free radical capture experiment determined that the main active species of the degradation reaction were e-, •O2- and •OH. The synergistic effect of the five components in the high entropy oxide strengthens lattice distortion and defects, increases oxygen vacancies, and thus has enhanced catalytic effect for TC-HCl degradation. This work shows that high entropy oxides have excellent catalytic performance for tetracycline organic pollutants, and it is speculated that high entropy oxides have good application prospects in the field of advanced oxidation technology for the degradation of organic pollutants.

Ultra-Broadband High-Entropy Oxide Absorber Layer for Enhanced Photodetector Performance.

A novel light-absorbing material of high-entropy oxide (HEO) has been synthesized using the hydrothermal method. The HEO has six metals, namely, Fe, Ni, Mn, Cr, Mg, and Cu. The obtained HEO light absorber is demonstrated to show unprecedented broadband absorption, ranging from 310 to 1400 nm. The photodetector having a structure of Ag/HEO/n-Si has been evaluated for its performance. Under the illumination of various light wavelengths, the photodetector exhibits a remarkably wide range of photoresponse from 365 to 1050 nm, giving wide-spectrum photocurrent densities in the order of 1 mA/cm2, a responsibility as high as 3.5 A/W (850 nm), and an external quantum efficiency (EQE) of more than 700% (850 nm), outperforming all of the reported oxide-based photodetectors. The superior device performance is attributed to the excellent light absorbance and EQE of the oxygen vacancy-containing HEO. Moreover, a number of tests, including the abrasion test, temperature endurance, acidic resistance, on-off switching cycling, and 3 dB bandwidth measurement, show the excellent reliability of the obtained HEO-based photodetector.

A High-Entropy-Oxides-Based Memristor: Outstanding Resistive Switching Performance and Mechanisms in Atomic Structural Evolution.

The application of high-entropy oxide (HEO) has attracted significant attention in recent years owing to their unique structural characteristics, such as excellent electrochemical properties and long-term cycling stability. However, the application of resistive random-access memory (RRAM) has not been extensively studied, and the switching mechanism of HEO-based RRAM has yet to be thoroughly investigated. In this study, HEO (Cr, Mn, Fe, Co, Ni)3 O4 with a spinel structure is epitaxially grown on a Nb:STO conductive substrate, and Pt metal is deposited as the top electrode. After the resistive-switching operation, some regions of the spinel structure are transformed into a rock-salt structure and analyzed using advanced transmission electron microscopy and scanning transmission electron microscopy. From the results of X-ray photoelectron spectroscopy and electron energy loss spectroscopy, only specific elements would change their valence state, which results in excellent resistive-switching properties with a high on/off ratio on the order of 105 , outstanding endurance (>4550 cycles), long retention time (>104 s), and high stability, which suggests that HEO is a promising RRAM material.