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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Bismuth Ferrite-Based Lead-Free High-Entropy Piezoelectric Ceramics

Hongtian Li,Jianwei Zhao,Yong Li,Longyu Chen,Xiaoxin Chen,Hailan Qin,Huanfu Zhou,Peifeng Li,Jinming Guo,Dawei Wang

Piezoelectric ceramics, as essential components of actuators and transducers, have captured significant attention in both industrial and scientific research. The “entropy engineering” approach has been demonstrated to achieve excellent performance in lead-based materials. In this study, the “entropy engineering” approach was employed to introduce the morphotropic phase boundary (MPB) into the bismuth ferrite (BF)-based lead-free system. By employing this strategy, a serial of novel “medium to high entropy” lead-free piezoelectric ceramics were successfully synthesized, namely (1–x)BiFeO3–x(Ba0.2Sr0.2Ca0.2Bi0.2Na0.2)TiO3 (BF–xBSCBNT, x = 0.15–0.5). Our investigation systematically examined the phase structure, domain configuration, and ferroelectric/piezoelectric properties as a function of conformational entropy. Remarkable performances with a largest strain of 0.50% at 100 kV/cm, remanent polarization ∼40.07 μC/cm2, coercive field ∼74.72 kV/cm, piezoelectric coefficient ∼80 pC/N, and d*33d33* ∼500 pm/V were achieved in BF–0.4BSCBNT ceramics. This exceptional performance can be attributed to the presence of MPB, coexisting rhombohedral and cubic phases, along with localized nanodomains. The concept of high-entropy lead-free piezoelectric ceramics in this study provides a promising strategy for the exploration and development of the next generation of lead-free piezoelectric materials.

研究领域: 材料科学 · 物理学
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Obtaining Low-Frequency and Broadband Absorbing Ferrite@C Microspheres through the High Entropy Engineering and Construction of Opened-Hollow Multi-Shell Architecture

Xiangyu Wang,Boyuan Cao,Hengbo Yin,Pengfei Yan,Tong Liu

The flexible manipulation of the position and type of metal cations in spinel ferrites gives the possibility of tuning its dielectric and magnetic properties, thus opening up broad design space for broadband and low-frequency absorption. However, there are still challenges in how to ensure that metal cations of diverse designs can be effectively introduced into the ferrite lattice to form homogeneous entropy-stable compounds, and further engender stable ferrite compounds with special multi-interface and hollow micro-nano structures to achieve lightweight and efficient performance. In this paper, the opened-hollow multi-shell high-entropy (FeCoNiZnMg)Fe 2 O 4 @C microspheres with a controllable carbon-coated triple-shell and entropy-stable ferrite composition are constructed. The designed hollow triple-shell structure enhances the magnetic interactions between the shells and regulates the magnetic domain structures and effective fields. The (FeCoNiZnMg)Fe 2 O 4 @C microspheres achieve an incredibly high absorption strengths (−60.5 dB) and wide effective absorption (9.3 GHz). Meanwhile, the high entropy effect effectively adjusts the anisotropic magnetic field size, significantly improving the low-frequency absorption of 4–8 GH band, far exceeding the performance of ferrite@C materials without forming a high-entropy phase. This unique hollow multi-shell ferrite@C composite based on high entropy strategy offers exciting prospects for rational composition and accurate structure construction for multi-interface polarization and lightweight design.

研究领域: 材料科学 · 电磁学
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JOURNAL OF APPLIED PHYSICS · 2023 ·Vol. 133 ·期 23 · IF 3.2

High-entropy enhanced microwave absorption in MAX phases

Shen Jibing,Zhang Min,Lin Shuai,Song Wenhai,Liu Huijun,Liu Qiangchun,Zhu Xuebin,Sun Yuping

The application of microwave absorption materials, which can effectively convert electromagnetic energy into thermal energy and/or other forms of energy, can effectively solve the increasingly serious electromagnetic pollution. As a type of promising microwave absorption material, ternary transition metal carbides/nitrides MAX phases possess layered structure and superior conduction loss capability. However, poor impedance matching and single polarization loss type seriously hinder their improvement of microwave absorption performance. High-entropy engineering is expected to be an effective strategy to address the above problems simultaneously. Herein, a series of low-, medium-, and high-entropy MAX phases with Ti 2 AlC structure were successfully synthesized and their structure, composition, and morphology were comprehensively characterized. High-entropy MAX phase (Ti 1/5 Zr 1/5 V 1/5 Nb 1/5 Ta 1/5 ) 2 AlC presents excellent microwave absorption performance with the optimal minimum reflection loss (RL min ) of −47 dB at 11.92 GHz (a thickness of 2.4 mm) and optimal effective absorption bandwidth of 3.92 GHz between 8.48 and 12.4 GHz (a thickness of 2.78 mm), which are better than those of our prepared low-/medium-entropy MAX phases as well as most of the other previously reported MAX phases. Such excellent microwave absorption performance of (Ti 1/5 Zr 1/5 V 1/5 Nb 1/5 Ta 1/5 ) 2 AlC is attributed to high-entropy engineering, which not only optimizes the impedance matching through regulating permittivity but also introduces more polarization loss type and amount. This work reveals that high-entropy engineering is not only a workable method to enhance the microwave absorption performance in MAX phases, but also an effective strategy to tailor the balance between impedance matching and loss capability through compositional design in single-phase systems.

研究领域: 材料科学 · 电磁学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

High-entropy engineering enables spinel oxides toward high-performance infrared radiation materials

Qifa Wan,Faming Zhang,Yifeng Xiong

High-entropy engineering, an emerging strategy, has recently received extensive attention for enhancing spinel oxides performance in diverse application fields. Herein, various novel non-equimolar spinel (Co,Mn,Fe,Cr,Ni,Al,Cu) 3 O 4 high-entropy oxides (HEOs) powders were successfully synthesized using a facile and scalable solid-state reaction method, which lied in the appropriate Cu cation content. The in-situ formed flaky alumina from potassium alum thermal decomposition, serving as the source of Al cation, promoted the formation of spinel HEOs powders instead of common reactive alumina powder. In particular, the infrared (IR) radiation performance of (Co 2/13 Mn 2/13 Fe 2/13 Cr 2/13 Ni 2/13 Al 2/13 Cu 1/13 ) 3 O 4 HEOs powder and coating was evaluated. This synthesized HEOs powder possessed a high IR emissivity of 0.885 in the near-IR band (0.78–2.5 µm) and good thermal stability. Notably, its IR emissivity was maintained at 0.874 with only a minimal loss of 1.2 % after high-temperature treatment. More importantly, this synthesized HEOs powder can be functioned as coating on substrates such as the Ti6Al4V alloy plate via the spraying method, exhibiting a superior IR emissivity of 0.925 and impressive radiant heat transfer capability. This work provides a good example of constructing high-performance spinel oxides through high-entropy engineering and holds great potential in developing energy-saving materials for high-temperature furnaces.

研究领域: 材料科学 · 能源工程 · 纳米技术
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

New Oxygen Regulation Strategy to Enhance the Oxygen Reduction Reaction of the Pr0.6Sr0.4Co0.2Fe0.8O3−δ Cathode through A-Site High-Entropy Engineering

Guobing Deng,Kai Kang,Yihui Liu,Chao Wang,Cheng Cheng Wang

Solid oxide fuel cell (SOFC) stands out as a highly promising energy conversion device, which can convert chemical energy directly into electrical energy. However, the decline in catalytic activity of the cathode becomes a major challenge for the commercialization of SOFC. Here, based on Pr0.6Sr0.4Co0.2Fe0.8O3−δ (PSCF), two novel A-site high-entropy perovskite cathodes, (Pr0.2Sr0.2La0.2Ba0.2Ca0.2)Co0.2Fe0.8O3−δ (PSLBCCF) and (Pr0.2Sr0.2La0.2Ba0.2Nd0.2)Co0.2Fe0.8O3−δ (PSLBNCF), are reported as high-catalyst-activity cathodes for SOFC. The synergistic action of high-entropy elements causes the valence state changes of the A-site Pr element and B-site Co–Fe element, which weakens the bonding energy of the metal element with O. It regulates the adsorption of surface oxygen and the dissociation of lattice oxygen, which enhances the transport of oxygen ions and greatly improves the oxygen reduction reaction and catalytic activity of the cathode. The polarization resistance (Rp) values of PSLBCCF and PSLBNCF cathodes at 750 °C are 0.083 and 0.072 Ω cm2, respectively, which are significantly lower than that of PSCF (0.122 Ω cm2). At 800 °C, the single cell supported by La0.8Sr0.2Ga0.8Mg0.2O3−δ as the electrolyte and high-entropy PSLBNCF as the cathode exhibited a power density of 561.09 mW cm–2. This study provides a new strategy for achieving excellent catalytic activity cathodes for SOFC.

研究领域: 材料科学 · 能源科学
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

Synergistically boosting high-temperature CO2 electrolysis performance via high-entropy engineering and anion doping strategy

Minglu Wang,Yun Da,Meiqiu Xie,Zheng Wang

Solid oxide electrolysis cell (SOEC) is recognized as a promising and efficient energy conversion technology by converting CO 2 into CO for achieving carbon neutrality. However, the cathode materials with insufficient electrocatalytic activity and stability greatly limit its large-scale commercial application. Herein, a synergistic strategy of high-entropy engineering and anion doping is proposed to develop a novel highly efficient and stable cathode material for CO 2 electrolysis in SOEC. Fluorine doped high-entropy perovskite La 0.6 Sr 0.4 Fe 0.3 Co 0.2 Ni 0.2 Mn 0.2 Mo 0.1 O 3-δ (LSFCNMM-F) is successfully synthesized to boost the CO 2 electrolysis performance. F doping can weaken the strength of metal-oxygen bond, increasing the concentration of oxygen vacancies, which significantly promotes the CO 2 adsorption and activation. Accordingly, F-doped high-entropy perovskite LSFCNMM-F cathode exhibits outstanding electrochemical performance and excellent stability for CO 2 electrolysis in SOEC. Compared to the pure high-entropy perovskite LSFCNMM, F-doped high-entropy perovskite LSFCNMM-F achieves 24.5 % improvement in current density with a remarkable value of 1.78 A/cm 2 at 1.5 V and 800 °C, surpassing most of the reported cathode materials in SOEC field. Moreover, the single cell with LSFCNMM-F cathode exhibits better long-term stability than that with pure high-entropy perovskite LSFCNMM cathode during 100 h operation at 1.2 V and 750 °C, owing to the inhabitation of Sr segregation on the electrode surface after F doping. The results from this study provide insights into the role of synergistic strategy for combining high-entropy engineering and anion doping in developing highly efficient and stable cathode for CO 2 electrolysis using SOEC technology.

研究领域: 材料科学 · 能源技术 · 化学工程
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Journal of Materials Chemistry A · 2025 ·Vol. 14 ·期 1 ·427-440 · IF 9.5

Synergistic high-entropy engineering in biphasic layered oxides enables high-rate sodium-ion cathodes

Jing Sun,Cailing Liu,Hongbo Huang,Xiaohong Liu,Meilan Xie,Lingling Liu,Juntong Huang,Dui Ma,Huan Liu,Peixun Xiong,Xiao Liang

Layered oxide cathodes for sodium-ion batteries (SIBs) are plagued by irreversible oxygen redox and structural degradation at high voltages, leading to severe capacity fade. To address this challenge, we synthesized a high-entropy biphasic oxide cathode, P2/O3-Na0.6Mn0.44Ni0.2Fe0.09Cu0.09Ti0.1Li0.04Mg0.04O2 (MNFCTLM) via a solid-phase method. The high-entropy composition effectively stabilizes the transition metal (TM)–O bonds, suppresses oxygen activity, and mitigates O2 precipitation. Concurrently, the biphasic structure offers additional Na+ migration channels, significantly enhancing ion diffusion kinetics. As a result, the MNFCTLM cathode delivers a specific capacity of 134.5 mAh g−1 at 0.2C and exhibits exceptional cycling stability, retaining 81.3% of its capacity after 200 cycles at 2C. It also achieves excellent rate performance (83.2 mAh g−1 at 20C) and exceptional air stability, retaining 86.4% of its initial capacity after seven days of air exposure. Ex situ XPS analysis revealed that, compared to the low-entropy P2-Na0.6Mn0.7Ni0.21Fe0.09O2 (MNF) cathode, MNFCTLM suppresses the formation of unstable On− species at high voltage. Ex situ XRD combined with DFT calculations further demonstrated the superior structural stability of MNFCTLM. In a full cell with a hard carbon anode, it demonstrates a high capacity of 160 mAh g−1 at 0.2C and retains 81.2% of its capacity after 200 cycles at 2C. This work not only presents a high-performance cathode for SIBs but also provides fundamental insight into stabilizing anionic redox through entropy engineering, offering a generalizable design strategy for advanced layered oxide electrodes.

研究领域: 材料科学 · 电化学 · 能源存储 · 无机化学 · 固态化学
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Energy & Environmental Science · 2025 · IF 30.8

High-entropy-induced CoO6 octahedral distortion for boosted oxygen evolution reaction at high temperature

Geng Zou,Hewei Liu,Tianfu Liu,Shaobo Han,Zijian Tan,Shaowei Zhang,Yige Guo,Jingcheng Yu,Xiaomin Zhang,Fang Lu,Yuefeng Song,Guoxiong Wang,Xinhe Bao

Modulating the distortion of BO6 octahedral plays a pivotal role in determining the physiochemical properties and electrocatalytic performance of the perovskite oxide (ABO3-δ). By tailoring the degree of octahedral tilting and bond angles, it could finely tune the electronic structure, oxygen vacancy formation, and ionic transport pathways within the perovskite lattice. Herein, we propose an efficient strategy to tune the BO6 (CoO6) octahedral distortion by the A-site high-entropy engineering in the Nd0.2Pr0.2La0.2Ba0.2Sr0.2CoO3-δ anode with the average Co-O-Co angle decreasing from 175° to 149°. Exsitu and in situ characterizations and density functional theory calculations reveal that the high-entropy-induced CoO6 octahedral distortion could shift the O 2p band center of the perovskite anode towards the Fermi level, and consequently activate the lattice oxygen and accelerate the transport of oxygen ions. Electrochemically, the CoO6-distorted Nd0.2Pr0.2La0.2Ba0.2Sr0.2CoO3-δ anode exhibits promoted high-temperature oxygen evolution reaction (OER) performance in solid oxide electrolysis cells (SOECs), with a high current density of 3.96 A·cm-2 at 1.5 V at 800 °C and stability for up to 600 hours, which is superior to most reported anode materials. This work discloses the impact of CoO6 octahedral distortion on high-temperature OER performance at atomic scale, and proposes an effective strategy for designing efficient and durable anodes of SOECs.

研究领域: 电催化 · 材料化学 · 能源化学 · 固态离子学 · 电化学 · 无机化学 · 高温材料科学
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