The single‐phase oxides with elemental complexity and compositional diversity, usually named high entropy oxides, feature homogeneously dispersed multi‐metallic elements in equiatomic concentration. The unusual properties of high entropy oxides endow their potential application in clean‐energy‐related electrocatalysis. However, the possible fundamental relationship between configuration entropy and the underlying catalytic mechanism is still not well understood and established. Herein, a high entropy perovskite cobaltate consisting of five equimolar metals in the B‐site (Mg, Mn, Fe, Co, and Ni) is employed as an electrocatalyst for oxygen evolution reaction (OER). The configuration entropy serves as an effective tool to promote the intrinsic activity of the Co reactive site and manipulate the OER mechanism. The high entropy cobaltate demonstrates a lower overpotential of 320 mV at a current density of 10 mA cm−2, outperforming other counterparts. The X‐ray spectroscopies disclose the synergistic charge‐exchange effect among different cations and the formation of a new oxygen hole state. Combinatorially computational and experimental results unveil the enigma that the high configuration entropy leads to the random occupation of cations, facilitates the surface reconstruction, and benefits the formation of stable surface oxygen vacancies. Owing to these merits, the O2 formation is found to be kinetically favorable via the lattice oxygen mechanism.

High Configuration Entropy Activated Lattice Oxygen for O2 Formation on Perovskite Electrocatalyst

High-entropy materials defy historical materials design paradigms by leveraging chemical disorder to kinetically stabilize novel crystalline solid solutions comprised of many endmembers. Formulational diversity results in local crystal structures that are seldom found in conventional materials that can strongly influence macroscopic physical properties. Thermodynamically prescribed chemical flexibility provides a means to tune such properties. Additionally, kinetic metastability results in many possible atomic arrangements, including both solid-solution configurations and heterogeneous phase assemblies, depending on synthesis conditions. Local disorder induced by metastability, and extensive cation solubilities allowed by thermodynamics combine to give many high-entropy oxide systems utility as electrochemical, magnetic, thermal, dielectric, and optical materials. Though high-entropy materials research is maturing rapidly, much remains to be understood and many compositions still await discovery, exploration, and implementation. This article is protected by copyright. All rights reserved 

High‐entropy oxides: Harnessing crystalline disorder for emergent functionality

Recently, superconductivity at about 9-15 K was discovered in Nd1-xSrxNiO2(Nd-112,x≈ 0.125-0.25) infinite-layer thin films, which has stimulated enormous interests in related rare-earth nickelates. Usually, the first step to synthesize this 112 phase is to fabricate theRNiO3(R-113,R: rare-earth element) phase, however, it was reported that the 113 phase is very difficult to be synthesized successfully due to the formation of unusual Ni3+oxidation state. And the difficulty of preparation is enhanced as the ionic radius of rare-earth element decreases. In this work, we report the synthesis and investigation on multiple physical properties of polycrystalline perovskites Sm1-xSrxNiO3(x= 0, 0.2) in which the ionic radius of Sm3+is smaller than that of Pr3+and Nd3+in related superconducting thin films. The structural and compositional analyses conducted by x-ray diffraction and energy dispersive x-ray spectrum reveal that the samples mainly contain the perovskite phase of Sm1-xSrxNiO3with small amount of NiO impurities. Magnetization and resistivity measurements indicate that the parent phase SmNiO3undergoes a paramagnetic-antiferromagnetic transition at about 224 K on a global insulating background. In contrast, the Sr-doped sample Sm0.8Sr0.2NiO3shows a metallic behavior from 300 K down to about 12 K, while below 12 K the resistivity exhibits a slight logarithmic increase. Meanwhile, from the magnetization curves, we can see that a possible spin-glass state occurs below 12 K in Sm0.8Sr0.2NiO3. Using a soft chemical reduction method, we also obtain the infinite-layer phase Sm0.8Sr0.2NiO2with square NiO2planes. The compound shows an insulating behavior which can be described by the three-dimensional variable-range-hopping model. And superconductivity is still absent in the polycrystalline Sm0.8Sr0.2NiO2.

https://iopscience.iop.org/article/10.1088/1361-648X/abfb90/pdf

Synthesis and physical properties of perovskite Sm1−x Sr x NiO3 (x = 0, 0.2) and infinite-layer Sm0.8Sr0.2NiO2 nickelates

Nucleation and epitaxy growth of high-entropy REBa2Cu3O7– (RE= Y, Dy, Gd, Sm, Eu) thin films by metal organic deposition

Abstract Compositionally complex materials have demonstrated extraordinary promise for structural robustness in extreme environments. Of these, the most commonly thought of are high entropy alloys, where chemical complexity grants uncommon combinations of hardness, ductility, and thermal resilience. In contrast to these metal-metal bonded systems, the addition of ionic and covalent bonding has led to the discovery of high entropy ceramics. These materials also possess outstanding structural, thermal, and chemical robustness but with a far greater variety of functional properties which enable access to continuously controllable magnetic, electronic, and optical phenomena. In this experimentally focused perspective, we outline the potential for high entropy ceramics in functional applications under extreme environments, where intrinsic stability may provide a new path toward inherently hardened device design. Current works on high entropy carbides, actinide bearing ceramics, and high entropy oxides are reviewed in the areas of radiation, high temperature, and corrosion tolerance where the role of local disorder is shown to create pathways toward self-healing and structural robustness. In this context, new strategies for creating future electronic, magnetic, and optical devices to be operated in harsh environments are outlined. 

pdf/high-entropy-ceramics-for-applications-in-extreme-tedegfzipb.pdf

High entropy ceramics for applications in extreme environments

In this study, we introduce the concept of high-entropy into high-temperature superconductors and report the successful synthesis of a series of high-entropy oxides, REBa2Cu3O7-δ (REBCO), with superconducting critical temperature (Tc) around 92 K. The superconductivity transition temperatures of these compounds are very close to that of the parent superconductor, YBa2Cu3O7-δ (YBCO). The temperatures of the zero-resistance appearing (Tczero), the critical current density (Jc) calculated from the hysteresis loop, and the irreversible fields (Hirr) of REBCO are not improved compared to that of YBCO. Our results indicate that the introduction of high-entropy elements with strong magnetic moments at RE site does not affect Tc, but may decrease other superconducting properties such as Jc, Tczero, and Hirr.

Structural and Physical Properties of High-Entropy REBa2Cu3O7-δ Oxide Superconductors

A series of copper thiospinels compounds, CuCo₂S_(4‐x)Se_x (x = 0, 0.2, 0.4, 0.6, 0.8), have been successfully synthesized by solid state reaction and their structure and magnetic properties have been studied. The Rietveld refinements of X‐Ray diffractions indicate that both the lattice constants and the nearest neighbor Cu‐Cu distances increase with increasing selenium doping. A weakly antiferromagnetic transition occurring at about 4 K is observed in CuCo₂S₄. Two antiferromagnetic transitions at about 3.5 K and 6 K are observed in selenium‐doped samples, which suggest that the exchange couplings associated with Cu‐S(Se)‐Cu and Cu‐Se(S)‐Cu, respectively, are responsible for the two antiferromagnetic transitions. Detailed analysis of the experimental results further indicate that the nearest‐neighbor molecular field coefficient is comparable to the next‐neighbor molecular field coefficient. We propose a reasonable model to explain this phenomenon.

/pdf/selenium-doping-induced-two-antiferromagnetic-transitions-in-35ol3k3yzd.pdf

Selenium doping induced two antiferromagnetic transitions in thiospinel compounds CuCo2S4-xSex (0 ≤ x ≤ 0.8)

Exchange Bias in Tetragonal Fe_1-xNi_xS Single Crystals with a Short-Range Antiferromagnetism

The evolution of spin-glass behavior in hexagonal Lu1-xCaxMnO3 single crystals

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Structural and Physical Properties of High-Entropy REBa2Cu3O7-δ Oxide Superconductors

Selenium doping induced two antiferromagnetic transitions in thiospinel compounds CuCo2S4-xSex (0 ≤ x ≤ 0.8)

Exchange Bias in Tetragonal Fe_1-xNi_xS Single Crystals with a Short-Range Antiferromagnetism

The evolution of spin-glass behavior in hexagonal Lu1-xCaxMnO3 single crystals