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ACS Nano · 2024 · IF 15.8

High-Entropy Rock-Salt Surface Layer Stabilizes the Ultrahigh-Ni Single-Crystal Cathode

Zhongxing Xu,Xinghan Chen,Wenguang Fan,Minzhi Zhan,Xulin Mu,Hongbin Cao,Xiaohu Wang,Haoyu Xue,Zhihai Gao,Yongzhi Liang,Jiajie Liu,Xinghua Tan,Feng Pan

Single-crystalline Ni-rich layered oxides are one of the most promising cathode materials for lithium-ion batteries due to their superior structural stability. However, sluggish lithium-ion diffusion kinetics and interfacial issues hinder their practical applications. These issues intensify with increasing Ni content in the ultrahigh-Ni regime (≥90%), significantly threatening the practical viability of the single-crystalline strategy for ultrahigh-Ni layered oxide cathodes. Herein, by developing a high-entropy coating strategy, we successfully constructed an epitaxial lattice-coherent high-entropy rock-salt layer (∼3 nm) via Zr and Al doping on the surface of the single-crystalline cathode LiNi0.92Co0.05Mn0.03O2 through an in situ modification process. The surface high-entropy rock-salt layer with tailored Ni valence and lattice coherence not only greatly improves lithium-ion diffusion kinetics but also suppresses interface parasitic reactions and surface structural degradations. The high-entropy surface layer-stabilized ultrahigh-Ni single-crystalline cathode (SC-Ni92-ZA) demonstrates significantly improved rate and cycling performances (127.5 mAh g–1 at 20C, capacity retention of 74.9% after 500 cycles at 1C) in a half-cell. The SC-Ni92-ZA exhibits a capacity retention of 87.1% after 600 cycles at 1C in a full-cell. This epitaxial lattice-coherent high-entropy coating strategy develops a promising avenue for developing high-capacity, long-life cathode materials.

研究领域: 材料科学 · 电化学 · 能源存储
✓ 已验证 DOI 高影响因子
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International Journal of Minerals Metallurgy and Materials · 2023 ·Vol. 30 ·期 11 ·2270-2279 · IF 4.8

FeCoNiCrMo high entropy alloy nanosheets catalyzed magnesium hydride for solid-state hydrogen storage

Zhong Tao,Zhang Haoyu,Song Mengchen,Jiang Yiqun,Shang Danhong,Wu Fuying,Zhang Liuting

The catalytic effect of FeCoNiCrMo high entropy alloy nanosheets on the hydrogen storage performance of magnesium hydride (MgH 2 ) was investigated for the first time in this paper. Experimental results demonstrated that 9wt% FeCoNiCrMo doped MgH 2 started to de-hydrogenate at 200°C and discharged up to 5.89wt% hydrogen within 60 min at 325°C. The fully dehydrogenated composite could absorb 3.23wt% hydrogen in 50 min at a temperature as low as 100°C. The calculated de/hydrogenation activation energy values decreased by 44.21%/55.22% compared with MgH 2 , respectively. Moreover, the composite’s hydrogen capacity dropped only 0.28wt% after 20 cycles, demonstrating remarkable cycling stability. The microstructure analysis verified that the five elements, Fe, Co, Ni, Cr, and Mo, remained stable in the form of high entropy alloy during the cycling process, and synergistically serving as a catalytic union to boost the de/hydrogenation reactions of MgH 2 . Besides, the FeCoNiCrMo nanosheets had close contact with MgH 2 , providing numerous non-homogeneous activation sites and diffusion channels for the rapid transfer of hydrogen, thus obtaining a superior catalytic effect.

研究领域: 材料科学 · 能源存储
✓ 已验证 DOI 高影响因子
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INORGANIC CHEMISTRY · 2024 · IF 4.3

Mechanochemical Synthesis of High-Entropy MOF-74 with Multiple Active Sites for CO2 Adsorption and Synergistic Conversion

Liang Ye,Ya Zhang,Siyang Jin,Chaohui Zhou,Junbao Pang,Yunjie Luo,Yuhang Yu,Wei Xu

Compared with monometallic metal–organic frameworks (MOFs), the synergistic effect of multiple metals significantly enhances the catalytic performance of the CO2 cycloesterification reaction, leading to improved CO2 adsorption and catalytic conversion capabilities. To investigate this concept, a high-entropy MOF-74 (HE-MOF-74) with a uniform distribution of five distinct metal ions (Zn2+, Mg2+, Ni2+, Co2+, and Cu2+) was successfully synthesized using a straightforward mechanical ball milling technique and comprehensively characterized (including structural, morphological, and physicochemical properties). The results reveal that HE-MOF-74 exhibits significantly increased specific surface area and CO2 adsorption capacity compared with those of monometallic MOF-74. The presence of multiple unsaturated metal centers as Lewis acid sites, oxygen atoms linking the metals, and ligand-based hydroxyl groups serving as base sites enable efficient immobilization of CO2 into cyclic carbonate. This study introduces a novel synthetic approach for the green and efficient production of HE-MOF-74 and proposes a new application for CO2 utilization.

研究领域: 材料科学 · 环境科学 · 催化化学
✓ 已验证 DOI PubMed 高影响因子
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Advanced Electronic Materials · 2022 ·Vol. 8 ·期 11 ·2200503 · IF 7.633

Achieving Excellent Energy Storage Properties in Fine-Grain High-Entropy Relaxor Ferroelectric Ceramics

Jian Guo,Wenrong Xiao,Xiaoyu Zhang,Ji Zhang,Jing Wang,Guangzu Zhang,Shan-Tao Zhang

ABO 3 -type high-entropy relaxor ferroelectric ceramics have rarely been studied in energy storage capacitor owing to easy formation of impurity phase. In this work, single phase (Bi 0.2 Na 0.2 Ba 0.2 Sr 0.2 Ca 0.2 )TiO 3 - x mol%PbO high-entropy ceramics are fabricated and investigated. The optimal composition of x = 2.0 shows a remarkable comprehensive energy storage performance with high recoverable energy density W rec = 8.2 J cm –3 , ultrahigh efficiency η = 92.2%, excellent temperature stability ( W rec = 4.4 J cm -3 ± 4%, η = 91% ± 3% within the range of 25–120 °C), and ultrafast discharge rate t 0.9 = 5.9 µs. Three key factors, low remnant polarization P r originating from high-entropy enhanced relaxation degree, high maximum polarization P m due to special electronic structure of Pb ion, and high electrical breakdown strength E b stemming from small grain size, are responsible for the improved energy storage properties. These results provide a novel strategy of developing high-entropy ceramics to optimize electrical performances including energy storage property.

研究领域: 材料科学 · 能源工程
✓ 已验证 DOI 高影响因子
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CERAMICS INTERNATIONAL · 2022 · IF 5.532

Large electrocaloric effect in two-step-SPS processed Pb(Sc0.25In0.25Nb0.25Ta0.25)O3 medium-entropy ceramics

Siyue Wei,Xue Chen,Guangzhi Dong,Laijun Liu,Qi Zhang,Biaolin Peng

Ferroelectric ceramic with a large electrocaloric ( EC ) effect at a very low electric field is very attractive in the next solid state refrigeration technology. In this work, two Pb(Sc 0.25 In 0.25 Nb 0.25 Ta 0.25 )O 3 (PSINT) medium-entropy ceramics were successfully synthesized by a spark plasma sintering (SPS) technology, including one-step-SPS processed and two-step-SPS processed samples. A large EC effect (△ T  ∼ 0.85 K) with a high EC strength (△ T /△ E  ∼ 0.021 K cm/kV) around room temperature are obtained at a very low electric field (∼40 kV/cm) in the two-step-SPS processed sample. Moreover, the working temperature range is very broad (∼120 K), which can be responsible for the high relaxation degree of the dielectric peak. It can be believed that the PSINT medium-entropy ceramics can be promising candidates for application in the next-generation EC cooling devices.

研究领域: 材料科学 · 物理学
✓ 已验证 DOI 高影响因子
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Microstructural and dielectric characteristics of A-site high-entropy oxide ceramics with a perovskite structure

Wenjing Qiao,Junwen Mei,Mei Bai,Yangfei Gao,Xiaopei Zhu,Yanhua Hu,Xiaojie Lou

High entropy oxides with interesting physical properties can be obtained by the design of A-site cations. Herein, a series of medium entropy and high entropy perovskite ceramics (Ba 0.25 Sr 0.25 Ca 0.25 Bi 0.25 )TiO 3 , (Ba 0.2 Sr 0.2 Ca 0.2 Bi 0.2 La 0.2 )TiO 3 , (Ba 0.2 Sr 0.2 Ca 0.2 Bi 0.2 Na 0.2 )TiO 3 and (Ba 0.2 Sr 0.2 Ca 0.2 La 0.2 Na 0.2 )TiO 3 were synthesized by the solid-state method, which selected various valence elements to achieve a single-phase structure and increase the lattice distortion. The microstructure indicated that the high-entropy ceramics exhibited the same macroscopic single perovskite while the local configuration is different. Mesoscopic results show that high entropy can adjust the polarization and relaxation of ferroelectrics , so as to optimize the energy storage performance. Meanwhile, the results manifest that grain boundaries, oxygen defects and relaxation can be changed by entropy configuration. Our work proves that the properties of high entropy ferroelectric materials can be regulated by different valence states of the elements in high entropy and explores the relevant mechanism, which provides a possible opportunity for the design and application of high-entropy dielectric materials with excellent properties.

研究领域: 材料科学 · 物理学
✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Phase compositions, microstructures, and microwave dielectric properties of novel high-entropy spinel-structured MAl2O4 ceramics

Zitao Shi,Xiao Zhang,Zeyu Zheng,Xiaodong Feng,Zixuan Fang,Bin Tang

High-entropy design for MgAl 2 O 4 spinel has rarely been reported. In this study, six novel high-entropy spinel-structured (HES) M Al 2 O 4 ceramics were prepared through the conventional solid-state reaction method. The effect of high-entropy design on the crystal structure, microscopic morphology, and microwave dielectric performance of HES ceramics was investigated based on X-ray diffraction (XRD), Raman spectra, and scanning/transmission electron microscopy (SEM/TEM). The analysis shows that the difference of one element among the high-entropy components can lead to an obvious variation in the lattice parameters, microstructures, and performance. The differences in microstructure, especially grain size, are the joint effects of particle size distribution, porosity, and composition. Specifically, (Mg 0.2 Mn 0.2 Co 0.2 Ni 0.2 Zn 0.2 )Al 2 O 4 (HES04) ceramic sintered at 1625 °C for 4 h exhibits superior properties: ε r =8.78 ± 0.03, Q× f =34,022 ± 910 GHz (@12.62 GHz), and τ f =−29.3 ± 0.6 ppm/°C. These results suggest that the high-entropy strategy is an effective method to tune the dielectric properties of MgAl 2 O 4 ceramic.

研究领域: 材料科学 · 无机化学
✓ 已验证 DOI 高影响因子
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POWDER METALLURGY · 2024 · IF 1.9

Effects of (ZrHfNbTaTiMo)C addition on microstructure and mechanical properties of WC-10Co cemented carbides

Xiao-Chun Deng,Guo-Hua Zhang

The WC-10Co cemented carbides containing (ZrHfNbTaTiMo)C high-entropy carbide with satisfactory comprehensive mechanical properties were successfully manufactured by conventional vacuum sintering. The influences of (ZrHfNbTaTiMo)C contents (0, 0.5, 1, 5, 10 wt.%) on the densification degree, microstructure, grain size and mechanical properties were investigated. The results showed that the addition of (ZrHfNbTaTiMo)C deteriorated the wettability between Co and WC, leading to a decline in relative density. (ZrHfNbTaTiMo)C inhibited the growth of WC grains, and the average grain size of WC continued to decrease with the increase of (ZrHfNbTaTiMo)C content. After adding (ZrHfNbTaTiMo)C, the hardness and toughness rose first and then descended. When the content of (ZrHfNbTaTiMo)C was 1 wt.%, the hardness and toughness reached the maximum value of 16.77 GPa and 10.45 MPa·m1/2, respectively. Moreover, the structure was a dual-grain structure, with many high-aspect-ratio rectangular grains in the sintered samples added by 0.5 wt.% and 1 wt.% (ZrHfNbTaTiMo)C. This special structure not only enhanced the hardness, but also compensated the loss of toughness. After doping 0.5 wt.% CeO2, the hardness decreased slightly, while the toughness increased to 12.42%.

研究领域: 材料科学 · 机械工程
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE · 2024 ·Vol. 59 ·期 22 ·9941-9951 · IF 3.5

Porous high-entropy (Zr0.25Hf0.25Nb0.25Ti0.25)C with high strength and uniform pore structure fabricated by freeze-casting

Zeng Dawei,Zhou Jiaxin,Wu Zhen,Sun Luchao,Wang Jingyang

Ultra-high temperature ceramics (UHTCs) are considered as promising thermal insulation materials applied in ultra-high temperature environments (> 2000 °C). However, the high thermal conductivity and high density limit their further development and application. Herein we adopt the strategies of introducing porous structure and high-entropy effect to solve the above problems. Thus porous high-entropy (Zr 0.25 Hf 0.25 Nb 0.25 Ti 0.25 )C ceramics were prepared. In order to obtain the uniform pore structure and high mechanical property, the camphene-based freeze-casting method was used in this study. The as-prepared porous samples exhibit high porosity of 92.01–73.57% and homogeneously interconnected pore structure with average pore size of 40.8–19.6 μm. Besides, this work realizes the aims of lightweight (0.65–2.15 g/cm 3 ) and low thermal conductivity (0.29–1.53 W/(m·K)). More importantly, porous samples still have the merit of high compressive strength (0.38–29.02 MPa) due to the even microstructure. The results show that highly porous high-entropy (Zr 0.25 Hf 0.25 Nb 0.25 Ti 0.25 )C with good overall properties can be an excellent candidate material for ultra-high temperature thermal insulation.

研究领域: 材料科学 · 陶瓷 · 热工学 · 机械工程
✓ 已验证 DOI 高影响因子
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Journal of Physical Chemistry Letters · 2014 · IF 6.687

Efficient and Energy-Saving CO2 Capture through the Entropic Effect Induced by the Intermolecular Hydrogen Bonding in Anion-Functionalized Ionic Liquids

Xiao Y. Luo,Fang Ding,Wen J. Lin,Yu Q. Qi,Hao R. Li,Cong M. Wang

A strategy for improving the capture of CO2 was developed through the entropic effect by tuning the geometric construction of anion-functionalized ionic liquids. Several kinds of anion-functionalized ionic liquids with the amino group at the para or ortho position were designed and applied for the capture of CO2, which indicates that the former exhibited both higher capacity and lower enthalpy, resulting in the efficient and energy-saving CO2 capture. Viscosity measurements, spectroscopic investigations, and quantum chemical calculations showed that such a unique behavior originated from the entropic effect, which was induced by the intermolecular hydrogen bonding in these ionic liquids. The entropic control for gas separation developed by this work provides an efficient strategy to both increased capacity and reduced enthalpy.

研究领域: 化学工程 · 环境科学 · 物理化学
✓ 已验证 DOI 高影响因子
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

High-temperature dimensional stability and radiation behavior of high-entropy rare earth tungstate ceramics

Jincheng Zhang,Liyan Xue,Wei Zhang,Yanyu Pan,Hongye Wang,Kaixian Wang,Heng Chen,Minzhong Huang,Fan Yang

Materials with high-temperature dimensional stability and resistance to radiation damage are receiving increasing attention in advanced nuclear energy systems . In this research, (Sm 0.2 Eu 0.2 Gd 0.2 Dy 0.2 A 0.2 ) 2 W 3 O 12 -type (A = Y, Tm,Ho) high-entropy ceramics is presented. The coefficients of thermal expansion of (Sm 0.2 Eu 0.2 Gd 0.2 Dy 0.2 Y 0.2 ) 2 W 3 O 12 (HE-RE 2 W 3 O 12 ) is 7.21 × 10 −6  K −1  at 300–1100K, which is the lowest among the three synthesized high-entropy ceramics and indicates good dimensional stability at high temperatures. After irradiation with Kr + fluence of 4.58 × 10 16 ions/cm 2 at 400 °C, both HE-RE 2 W 3 O 12 and Gd 2 W 3 O 12 maintained crystalline, but the lattice volume expansion rate of HE-RE 2 W 3 O 12 (0.71 %) is much lower than that of Gd 2 W 3 O 12 (1.49 %). Additionally, in the post-irradiated HE-RE 2 W 3 O 12 , the Raman spectra vibration peak remained unchanged and no radiation-induced segregation was observed. Nanoindentation tests displayed that the degradation of hardness and elastic modulus in HE-RE 2 W 3 O 12 is rarely degrade. Overall, these results provide new insights for research on advanced nuclear materials in the future.

研究领域: 材料科学 · 核能工程
✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Structural, thermophysical, mechanical and electrical properties of equimolar five-principal element fluorite-structured high-entropy oxides

Xinyu Ping,Qingqing Yang,Bin Meng,Zhiyuan Ma,Xiaoyu Pan

Four kinds of high-entropy oxides (HEOs) with compositions of Y 0.2 Zr 0.2 Hf 0.2 Ce 0.2 X 0.2 O 2−δ (X = La, Nd, Gd, Dy, abbreviated as HEO-La, Nd, Gd, Dy, respectively) are synthesized by solid-state-reaction method combined with conventional sintering in air atmosphere at 1600 °C for 10 h. These HEOs have a fluorite-structured phase with homogeneous element distribution. The thermal conductivity ( κ ) of these four samples is in 1.68–2.18 W m −1 K −1 in 25–900 °C. At 800 °C and 900 °C, the κ value of HEO-Gd is lower than those of the HEO-La, Nd, Dy, yttria-stabilized zirconia (YSZ) and some other HEOs with various crystal structures ((Gd 0.2 Dy 0.2 Ho 0.2 Er 0.2 Tm 0.2 )Ta 3 O 9 , (La 0.25 Eu 0.25 Gd 0.25 Yb 0.25 ) 2 Zr 2 O 7 , (Sm 0.2 Dy 0.2 Ho 0.2 Er 0.2 Yb 0.2 )NbO 4 , Hf 0.25 Zr 0.25 Ce 0.25 Gd 0.125 Ca 0.125 O 2-δ and Sr(Y 0.2 Sm 0.2 Gd 0.2 Dy 0.2 Yb 0.2 ) 2 O 4 ). The sample of HEO-Gd has the highest thermal expansion coefficient (CTE) (12.1 × 10 −6 K −1 ) and fracture toughness ( K IC ) (2.5 MPa m 1/2 ) among HEO-La, Nd, Gd, Dy. Its K IC value is higher than those of other HEOs mentioned above. In addition, HEO-Gd exhibits a better oxygen barrier property compared with YSZ in 450–700 °C. These results indicate that HEO-Gd is a promising candidate as high-temperature thermal insulation ceramic.

研究领域: 材料科学 · 无机非金属材料 · 高温陶瓷 · 热障涂层 · 固态离子学
✓ 已验证 DOI 高影响因子
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