High‐Entropy Sulfides as Electrode Materials for Li‐Ion Batteries (Adv. Energy Mater. 8/2022)

Li, Gang; Wang, Kai; Sarkar, Abhishek; Njel, Christian; Karkera, Guruprakash; Wang, Qingsong; Azmi, Raheleh; Fichtner, Maximilian; Hahn, Horst; Schweidler, Simon; Breitung, Ben

doi:10.1002/aenm.202270030

Cited by 21 publications

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“…High‐entropy alloys are generally described as a solid solution containing at least five principal metals, and each metal possess a molar ratio in the range of 5–35%. [ 1b ] This notion has been extended to create entropy‐stabilized functional oxide ceramics. [ 6a ] When the increase in entropy exceeds the increase in enthalpy for a particular system, the configurational entropy increases, resulting in a lower Gibbs free energy and stable crystal structures.…”

Section: Resultsmentioning

confidence: 99%

“…The high‐entropy (HE) design forces multiple principal elements into a single‐phase structure to afford 1) high configurational entropy and 2) a specific union of interactions according to the stoichiometry and type of incoming elements. [ 1 ] The addition of numerous main metal elements into high‐entropy alloys (HEAs) have been popular since their discovery in 2004. [ 2 ] This has provided a vast combinatorial space for the exploration of new materials with unexplored abnormal functionalities.…”

Section: Introductionmentioning

confidence: 99%

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High‐Entropy Enhanced Microwave Attenuation in Titanate Perovskites

et al. 2023

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The addition of numerous main metal elements into highentropy alloys (HEAs) have been popular since their discovery in 2004. [2] This has provided a vast combinatorial space for the exploration of new materials with unexplored abnormal functionalities. In general, four core factors, namely, sluggish diffusion, configurational entropy, lattice distortion, and cocktail effects, affect the crystal structure and properties of HEAs. [3] Since 2015, the concept of high entropy has been successfully expanded to include oxides. [4] Similar to HEAs, high-entropy oxides (HEOs) are defined as compositions consisting of oxygen and more than five metal cations in equimolar or near equimolar ratios in the range of 5-35% atomic concentration. [5] HEOs are rapidly emerging as delicate functional constituents that offer excellent compositional flexibility that permits the stabilization of numerous compositions with various crystal structures (e.g., rock-salt, spinel, fluorite, perovskite, and pyrochlore phases). [6] Consequently, HEOs present numerous attractive functional properties, such as high ionic conductivity; [7] superior storage capacity retention and good stable cycles of Li battery; [8] low thermal conductivity and good thermal stability; colossal dielectric constant; [9] and novel magnetic phenomena. [10] However, a deep understanding of their microstructures has yet to emerge. Thus, it is extremely urgent to learn more about the microstructure of HEOs to further understand their anomalous High-entropy oxides (HEOs), which incorporate multiple-principal cations into single-phase crystals and interact with diverse metal ions, extend the border for available compositions and unprecedented properties. Herein, a high-entropy-stabilized (Ca 0.2 Sr 0.2 Ba 0.2 La 0.2 Pb 0.2 )TiO 3 perovskite is reported, and the effective absorption bandwidth (90% absorption) improves almost two times than that of BaTiO 3 . The results demonstrate that the regulation of entropy configuration can yield significant grain boundaries, oxygen defects, and an ultradense distorted lattice. These characteristics give rise to strong interfacial and defect-induced polarizations, thus synergistically contributing to the dielectric attenuation performance. Moreover, the large strains derived from the strong lattice distortions in the high-entropy perovskite offer varied transport for electron carriers. The high-entropy-enhanced positive/negative charges accumulation around grain boundaries and strain-concentrated location, quantitatively validated by electron holography, results in unusual dielectric polarization loss. This study opens up an effective avenue for designing strong microwave absorption materials to satisfy the increasingly demanding requirements of advanced and integrated electronics. This work also offers a paradigm for improving other interesting properties for HEOs through entropy engineering.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

High‐Entropy Enhanced Microwave Attenuation in Titanate Perovskites

et al. 2023

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“…[ 2 ] The principal concept of high entropy alloys was extended to high entropy oxides (HEO), sulfides, fluorites, and carbides in recent years. [ 3–7 ] Up to date, high entropy oxides have been demonstrated as a promising material class, since unique and tailored material properties can be designed, such as unusually high dielectric constants, [ 8 ] enhanced and stable lithium ion transport and storage properties, [ 9 ] and exceptional (electro‐) catalytic activities. [ 10,11 ] These remarkable and unprecedented performances have been generally ascribed to the numerous possible interactions (synergistic effects) of the constituting elements, which will modify the corresponding electronic structure and may induce charge carrier transfer among the crystallographic sites, [ 12 ] and thus, enables a wide range of novel applications of high entropy oxides with tailored (electronic) properties.…”

Section: Introductionmentioning

confidence: 99%

Sol‐Gel‐Derived Ordered Mesoporous High Entropy Spinel Ferrites and Assessment of Their Photoelectrochemical and Electrocatalytic Water Splitting Performance

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Waheed

Lauterbach

et al. 2023

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The novel material class of high entropy oxides with their unique and unexpected physicochemical properties is a candidate for energy applications. Herein, it is reported for the first time about the physico‐ and (photo‐) electrochemical properties of ordered mesoporous (CoNiCuZnMg)Fe2O4 thin films synthesized by a soft‐templating and dip‐coating approach. The A‐site high entropy ferrites (HEF) are composed of periodically ordered mesopores building a highly accessible inorganic nanoarchitecture with large specific surface areas. The mesoporous spinel HEF thin films are found to be phase‐pure and crack‐free on the meso‐ and macroscale. The formation of the spinel structure hosting six distinct cations is verified by X‐ray‐based characterization techniques. Photoelectron spectroscopy gives insight into the chemical state of the implemented transition metals supporting the structural characterization data. Applied as photoanode for photoelectrochemical water splitting, the HEFs are photostable over several hours but show only low photoconductivity owing to fast surface recombination, as evidenced by intensity‐modulated photocurrent spectroscopy. When applied as oxygen evolution reaction electrocatalyst, the HEF thin films possess overpotentials of 420 mV at 10 mA cm−2 in 1 m KOH. The results imply that the increase of the compositional disorder enhances the electronic transport properties, which are beneficial for both energy applications.

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“…To better evaluate the performance improvement of such configurational entropy evolution and certify its significance worked in metal‐phosphorus, we take the well‐designed HEM‐5555 products to compare with recent published work on anode materials. As shown in Figure 4f, when compared to unitary Si, [ 33 ] P, [ 34 ] Ge, [ 35 ] binary GeP 3, , [ 36 ] GeMg, [ 37 ] SiP 2 , [ 38 ] SiO x /TiO 2 , [ 39 ] ternary ZnSnS 3 , [ 40 ] Cu 6 Sn 5 @SnO 2 , [ 41 ] ZZFO, [ 42 ] and quaternary LiLaTiNiO, [ 43 ] NiCoV 2 O 8 , [ 44 ] (Mg 0.2 Co 0.2 Ni 0.2 Cu 0.2 Zn 0.2 )O, [ 45 ] and (FeMnNiCoCr)S 2 [ 46 ] , those well‐designed Zn x Ge y Cu z Si w P 2 HEM solid solutions surpass all the above materials owing to its larger configurational entropy triggered higher reversibility (ICE = 93%) and excellent rate performances, greatly proving the efficiency and significance of high entropy concept in LIBs.…”

Section: Resultsmentioning

confidence: 99%

Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries

et al. 2023

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The high‐entropy materials (HEM) have attracted increasing attention in catalysis and energy storage due to their large configurational entropy and multiunique properties. However, it is failed in alloying‐type anode due to their Li‐inactive transition‐metal compositions. Herein, inspired by high‐entropy concept, the Li‐active elements instead of transition‐metal ones are introduced for metal‐phosphorus synthesis. Interestingly, a new ZnxGeyCuzSiwP2 solid solution is successfully synthesized as proof of concept, which is first verified to cubic system in F‐43m. More specially, such ZnxGeyCuzSiwP2 possesses wide‐range tunable region from 9911 to 4466, in which the Zn0.5Ge0.5Cu0.5Si0.5P2 accounts for the highest configurational entropy. When served as anode, ZnxGeyCuzSiwP2 delivers large capacity (>1500 mAh g−1) and suitable plateau (≈0.5 V) for energy storage, breaking the conventional view that HEM is helpless for alloying anode due to its transition‐metal compositions. Among them, the Zn0.5Ge0.5Cu0.5Si0.5P2 exhibits the highest initial coulombic efficiency (ICE) (93%), Li‐diffusivity (1.11 × 10−10), lowest volume‐expansion (34.5%), and best rate performances (551 mAh g−1 at 6400 mA g−1) owing to its largest configurational entropy. Possible mechanism reveals the high entropy stabilization enables good accommodation of volume change and fast electronic transportation, thus supporting superior cyclability and rate performances. This large configurational entropy strategy in metal‐phosphorus solid solution may open new avenues to develop other high‐entropy materials for advanced energy storage.

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High‐Entropy Sulfides as Electrode Materials for Li‐Ion Batteries (Adv. Energy Mater. 8/2022)

Cited by 21 publications

References 0 publications

High‐Entropy Enhanced Microwave Attenuation in Titanate Perovskites

High‐Entropy Enhanced Microwave Attenuation in Titanate Perovskites

Sol‐Gel‐Derived Ordered Mesoporous High Entropy Spinel Ferrites and Assessment of Their Photoelectrochemical and Electrocatalytic Water Splitting Performance

Understanding the Configurational Entropy Evolution in Metal‐Phosphorus Solid Solution for Highly Reversible Li‐Ion Batteries

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