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Magnetic and dielectric properties of low-loss MnZn ferrites with wide temperature stability 具有宽温度稳定性的低损耗锰锌铁氧体的磁性和介电特性
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-09-13 DOI: 10.1111/jace.20137
Yao Ying, Guo Chen, Zhaocheng Li, Jingwu Zheng, Jing Yu, Liang Qiao, Wangchang Li, Juan Li, Naoki Wakiya, Masahiro Yamaguchi, Shenglei Che

To meet the needs for higher energy efficiency and a wide operating temperature range of electric vehicles, the low-loss MnZn ferrites in a wide temperature range have been developed by optimizing the Fe content and the oxygen partial pressure (PO2) during the sintering process in this work. For the optimal sample, power loss at 300 kHz/100mT is 204 kW/m3 at 25°C and remains below 290 kW/m3 in the wide temperature range from -10 to 120°C. The loss separation method was employed to clarify the effects of the Fe content and PO2 on power loss. The equivalent circuit model has been employed to fit the complex impedance and it is found that the increase of PO2 enhances both the grain resistance Rg and the grain boundary resistance Rgb. The enhancement of Rgb is mainly responsible for the reduction of eddy current loss and consequently power loss. Dielectric permittivity is as large as about 15000 in this series of samples due to the electric polarization at the rich grain boundaries. Dielectric loss is very low between -50 and 150°C and has little contribution to the energy loss.

为了满足电动汽车对更高能效和更宽工作温度范围的需求,本研究通过优化烧结过程中的铁含量和氧分压(PO2),开发出了宽温度范围内的低损耗锰锌铁氧体。对于最佳样品,300 kHz/100mT 的功率损耗在 25°C 时为 204 kW/m3,在 -10 至 120°C 的宽温度范围内保持在 290 kW/m3 以下。采用损耗分离法来阐明铁含量和 PO2 对功率损耗的影响。采用等效电路模型拟合复阻抗,发现 PO2 的增加会增强晶粒电阻 Rg 和晶界电阻 Rgb。Rgb 的增强是涡流损耗减少的主要原因,因此也是功率损耗减少的主要原因。由于富晶粒边界的电极化,该系列样品的介电常数高达约 15000。介电损耗在 -50 至 150°C 之间非常低,对能量损耗的影响很小。
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引用次数: 0
Evaluation of crack initiation load of silica glass surfaces formed during subcritical crack growth 评估亚临界裂纹生长过程中形成的硅玻璃表面的裂纹起始载荷
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-09-13 DOI: 10.1111/jace.20115
Jun Endo, Tomomi Sekine, Souta Shimizu, Satoshi Yoshida

The crack initiation load of freshly fractured surfaces for silica glass was evaluated with ball indentation. The fracture surfaces were formed during subcritical crack growth in the regions I, II, and III of the stress intensity factor (KI)—crack velocity (V) curve. From the KIV curve, we linked the obtained fracture surfaces with the ones in the regions I, II, and III. It was found that the crack-forming probability was the lowest for the fracture surface formed in the region III of the KIV curve. In order to understand the controlling factors of the crack formation, some properties which are topography, relative nonbridging oxygens (NBO), hydrogen concentrations, and Si–O three- or four-membered ring structures, of the fracture surfaces were measured by atomic force microscopy, X-ray photoelectron spectroscopy, dynamic secondary ion mass spectroscopy, and Raman spectroscopy, respectively. No distinct difference in NBO and hydrogen concentrations nor the ring structures were found among the fracture surfaces formed in different regions in the KIV curve. The peak-to-valley height of the fracture surface, however, decreased with increasing crack velocity. It is concluded that the roughness or topography of the freshly fractured surface is one of the controlling factors which reduce the intrinsic strength of silica glass.

采用球压痕法评估了硅玻璃新断裂表面的裂纹起始载荷。断裂面是在应力强度因子(KI)-裂纹速度(V)曲线的 I、II 和 III 区域的亚临界裂纹生长过程中形成的。根据 KI-V 曲线,我们将获得的断裂面与 I、II 和 III 区域的断裂面联系起来。结果发现,在 KI-V 曲线区域 III 中形成的断裂面的裂纹形成概率最低。为了了解裂纹形成的控制因素,我们分别用原子力显微镜、X 射线光电子能谱、动态二次离子质谱和拉曼光谱测量了断裂表面的形貌、相对非杂氧 (NBO)、氢浓度、Si-O 三元或四元环结构等特性。在 KI-V 曲线的不同区域形成的断裂面,其 NBO 和氢浓度以及环状结构均无明显差异。然而,断裂面的峰谷高度随着裂纹速度的增加而降低。由此得出结论,新断裂表面的粗糙度或形貌是降低硅玻璃内在强度的控制因素之一。
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引用次数: 0
Strategies to improve oxidation resistance of MgO–C refractories by decreasing oxygen potential through MgSiN2 通过 MgSiN2 降低氧势以提高 MgO-C 耐火材料抗氧化性的策略
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-09-13 DOI: 10.1111/jace.20114
Fanqiang Meng, Yixin Luo, Zhenglong Liu, Chao Yu, Chengji Deng, Jun Ding

MgO–C refractories are of paramount importance in the converter side blowing system, requiring outstanding oxidation resistance under harsh conditions including high temperature, oxygen atmosphere, and high-speed airflow. In this study, MgSiN2 phase reconstruction was used to improve the oxidation resistance of MgO–C refractories, as well as the mechanical properties and oxidation resistance of MgO–C refractories were evaluated. The results indicated that the cold modulus of rupture of the sample with 9 wt% MgSiN2 was increased by 93.3% compared with the MgO–C refractories without MgSiN2. After oxidation tests, the oxidation index and rate constant (k) of the sample with 9 wt% MgSiN2 were reduced by 38.9% and 35.3%. Furthermore, incorporating MgSiN2 facilitated the formation of layered dense structures consisting of plate-like Mg-Sialon and MgO–Mg2SiO4–MgAl2O4. This structural optimization effectively inhibited oxygen diffusion and reaction within the material, resulting in gradual oxygen potential mitigation.

氧化镁-碳耐火材料在转炉侧吹灰系统中至关重要,需要在高温、氧气环境和高速气流等恶劣条件下具有出色的抗氧化性。本研究采用 MgSiN2 相重构来提高 MgO-C 耐火材料的抗氧化性,并对 MgO-C 耐火材料的机械性能和抗氧化性进行了评估。结果表明,与不含 MgSiN2 的 MgO-C 耐火材料相比,含 9 wt% MgSiN2 的样品的冷断裂模量提高了 93.3%。经过氧化测试,含有 9 wt% MgSiN2 的样品的氧化指数和速率常数(k)分别降低了 38.9% 和 35.3%。此外,MgSiN2 的加入还促进了由板状 Mg-Sialon 和 MgO-Mg2SiO4-MgAl2O4 组成的层状致密结构的形成。这种结构优化有效地抑制了材料内部的氧扩散和反应,从而逐步降低了氧电势。
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引用次数: 0
Thermal shock behavior of andalusite-based refractories: Microstructural investigation of crack bridging and grain-matrix interactions 基于安达卢西亚石的耐火材料的热冲击行为:裂纹桥接和晶粒-基质相互作用的微观结构研究
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-09-13 DOI: 10.1111/jace.20117
Dominik Hahn, Jong-Won Shin, David Tissen, Almuth Sax, Peter Quirmbach

Andalusite-based refractories are characterized by superior thermal shock resistance. Although the demand for alternative raw materials is increasing, it is proving difficult to replicate the thermal shock behavior of andalusite with alternative materials. The physico-mechanical properties of andalusite refractories are well-studied. However, comprehensive chemical and microstructural analysis is still needed to fully understand factors influencing the thermal shock resistance. This investigation highlights the use of complementary microstructural techniques (3D digital microscopy, scanning electron microscopy–energy-dispersive X-ray spectroscopy, and micro-X-ray fluorescence) to analyze crack propagation as well as glass bridge formation and composition in aluminosilicate-based refractory castables. Andalusite-based refractories are compared with chamotte 45 and chamotte 60, before and after a thermal shock, as well as after an additional firing. Factors influencing the thermal shock resistance of aluminosilicate refractory castables include (1) crack shape, size, occurrence, and propagation (2) glass bridge formation, size, occurrence, and composition, and (3) aggregate-matrix interactions.

安达卢西亚石基耐火材料具有优异的抗热震性。尽管对替代原材料的需求不断增加,但事实证明,用替代材料来复制安达卢西亚石的抗热震性能十分困难。安达卢瑟石耐火材料的物理机械性能已得到充分研究。然而,要充分了解影响抗热震性的因素,还需要进行全面的化学和微观结构分析。本研究强调使用互补的微观结构技术(三维数字显微镜、扫描电子显微镜-能量色散 X 射线光谱和微 X 射线荧光)来分析铝硅酸盐基耐火浇注料中的裂纹扩展、玻璃桥形成和成分。在热冲击前后以及额外焙烧后,将安达卢硅酸盐基耐火材料与 Chamotte 45 和 Chamotte 60 进行了比较。影响铝硅酸盐耐火浇注料抗热震性的因素包括:(1) 裂纹的形状、大小、出现和扩展;(2) 玻璃桥的形成、大小、出现和组成;以及 (3) 骨料与基质之间的相互作用。
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引用次数: 0
Resolving the hardness–toughness trade-off dilemma of metal/ceramic multilayer films by introducing gradient structure 通过引入梯度结构解决金属/陶瓷多层薄膜的硬度-韧性权衡难题
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-08-29 DOI: 10.1111/jace.20112
Wentao Zhang, Kaiwen Wang, Rui Zhang, Xinlei Gu, Jingjie Pan, Zhongzhen Wu, Xiyao Zhang, Wen Mao, Kan Zhang

Equal-period modulated metal/ceramic multilayers have shown promise in enhancing the toughness of ceramic thin films. However, this toughness enhancement typically comes at the sacrifice of hardness, limiting their potential applications. To tackle this issue, this study designed and fabricated two gradient-structured multilayer variations using Ta/TaB2: one with a higher ceramic layer fraction near the surface (M2) and the other with a converse structure (M3). A conventional equal modulation period Ta/TaB2 multilayer film (M1) served as a reference. M2 exhibited superior performance, with a 30% hardness increase and significant toughness enhancement compared to M1. Conversely, M3 experienced failure due to excessive thermal stress from its unique gradient structure. Finite element simulations revealed that M2's structure could alleviate in-plane stress and enhance loading uniformity, thus enhancing the film's toughness. These findings suggest that a well-designed gradient structure holds promise for concurrently improving the hardness and toughness of metal/ceramic multilayer films.

等周期调制金属/陶瓷多层膜在提高陶瓷薄膜的韧性方面大有可为。然而,这种韧性的增强通常是以牺牲硬度为代价的,从而限制了它们的潜在应用。为了解决这个问题,本研究使用 Ta/TaB2 设计并制造了两种梯度结构的多层变化:一种是靠近表面的陶瓷层比例较高 (M2),另一种是相反的结构 (M3)。传统的等调制周期 Ta/TaB2 多层薄膜(M1)作为参照。与 M1 相比,M2 表现出更优越的性能,硬度提高了 30%,韧性显著增强。相反,M3 则由于其独特的梯度结构产生了过大的热应力而失效。有限元模拟显示,M2 的结构可以减轻面内应力,提高加载均匀性,从而增强薄膜的韧性。这些发现表明,设计良好的梯度结构有望同时提高金属/陶瓷多层薄膜的硬度和韧性。
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引用次数: 0
Influence of cerium addition and redox state on silicate structure and viscosity 铈添加和氧化还原状态对硅酸盐结构和粘度的影响
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-08-29 DOI: 10.1111/jace.20113
Adrien Donatini, Luiz Pereira, Donald B. Dingwell, Kai-Uwe Hess, Dirk Müller, Laurent Cormier, Daniel R. Neuville

The viscosities of Ce-free and Ce-bearing (∼1.3 mol%, ∼6.5 wt.% Ce2O3) soda lime silicate (window glass) melts were measured with respect to oxidation state. Experiments were performed isothermally using a concentric-cylinder viscometer on melts equilibrated with successively reducing CO–CO2 gas mixtures within a gas tight vertical tube furnace at 1 atm. Viscosity measurement and sampling were performed at the end of each melt reduction step. Further, viscosities in the glass transition temperature range were estimated using the shift factor method applied to glass transition temperature values determined using differential scanning calorimetry (DSC) measurements on quenched glasses. The Ce speciation at each stepwise melt reduction was probed using Ce L3-edge X-ray absorption near-edge structure (XANES) spectroscopy, while structural information upon Ce addition and reduction was provided by Raman spectroscopy. The viscosities of these materials remain constant at this level of Ce addition and do not vary significantly with redox state at high temperature. Conversely, viscosity values in the glass transition temperature range increase upon both Ce addition and reduction. Our analysis, based on the glass composition analyses obtained via electron probe microanalyzer (EPMA), viscosity calculations, and observations of silicate structural changes, leads to the conclusion that the observed viscosity increase around the glass transition temperature is explained by the high ionic field strength of Ce ions as well as the polymerization behavior of the silicate matrix occurring during reduction of Ce. Because of its low concentration, resulting from its low solubility, Ce redox changes exert only minimal effects on the viscosity of this melt.

测量了不含 Ce 和含 Ce(1.3 mol%∼6.5 wt.% Ce2O3)的钠钙硅酸盐(窗玻璃)熔体的粘度与氧化态的关系。实验采用同心圆筒粘度计,在 1 atm 的气密性垂直管式炉中,用连续还原的 CO-CO2 混合气体对熔体进行等温平衡。粘度测量和取样在每个熔体还原步骤结束时进行。此外,玻璃转化温度范围内的粘度是通过对淬火玻璃进行差示扫描量热法(DSC)测量所确定的玻璃转化温度值,采用移动因子法进行估算的。使用 Ce L3-edge X 射线吸收近缘结构 (XANES) 光谱法探测了每一步熔融还原时的 Ce 标示,而拉曼光谱法则提供了添加和还原 Ce 时的结构信息。这些材料的粘度在这一添加量下保持不变,并且在高温下不会随氧化还原状态发生显著变化。相反,玻璃转化温度范围内的粘度值在添加和还原 Ce 时都会增加。我们根据电子探针显微分析仪(EPMA)获得的玻璃成分分析、粘度计算和硅酸盐结构变化的观察结果进行分析,得出结论认为,在玻璃化温度附近观察到的粘度增加是由于 Ce 离子的高离子场强以及在 Ce 还原过程中硅酸盐基质的聚合行为造成的。由于铈的溶解度低,铈的氧化还原变化对这种熔体的粘度影响很小。
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引用次数: 0
The wettability of pure liquid aluminum on oxide substrates 氧化物基底上纯铝液的润湿性
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-08-28 DOI: 10.1111/jace.20103
Xingwen Wei, Beate Fankhänel, Wei Zhao, Anton Perminov, Enrico Storti, Mengke Liu, Guojun Ma, Olga Fabrichnaya, Alexandros Charitos, Olena Volkova

Oxide particles are considered to be one of the reasons for the stability of cellular porous Al foam. Thus, the contact angle (ө) of molten pure aluminum on oxide substrates, including Al2O3, CaO·2Al2O3 (CA2), CaO·6Al2O3 (CA6), mullite (3Al2O3·2SiO2), and SiO2 was measured in a vacuum heating microscope at a temperature of 950°C to determine the value of wettability of molten aluminum on various oxides. Thereafter, the measured contact angles followed the tendency as mullite (155°) > CA6 (152°) > MgAl2O4 (151°) > Al2O3 (149°) > SiO2 (124°) > CA2 (100°). Furthermore, the cross-sectional area between molten aluminum and substrates was thoroughly analyzed, and the reaction products, such as the Al2O3 layer at the interface, have been detected. Thermo-Calc, with the combination of available databases, was used to perform thermodynamic simulations and to discuss and predict possible reactions under the current experimental conditions.

氧化物颗粒被认为是蜂窝状多孔铝泡沫稳定性的原因之一。因此,在真空加热显微镜中,在 950°C 的温度下测量了熔融纯铝在氧化物基底(包括 Al2O3、CaO-2Al2O3 (CA2)、CaO-6Al2O3 (CA6)、莫来石(3Al2O3-2SiO2)和 SiO2)上的接触角 (ө),以确定熔融铝在各种氧化物上的润湿性值。此后,所测得的接触角呈以下趋势:莫来石(155°)> CA6(152°)> MgAl2O4(151°)> Al2O3(149°)> SiO2(124°)> CA2(100°)。此外,还对熔融铝和基底之间的横截面积进行了深入分析,并检测到了反应产物,如界面上的 Al2O3 层。Thermo-Calc 结合现有数据库进行了热力学模拟,并对当前实验条件下可能发生的反应进行了讨论和预测。
{"title":"The wettability of pure liquid aluminum on oxide substrates","authors":"Xingwen Wei,&nbsp;Beate Fankhänel,&nbsp;Wei Zhao,&nbsp;Anton Perminov,&nbsp;Enrico Storti,&nbsp;Mengke Liu,&nbsp;Guojun Ma,&nbsp;Olga Fabrichnaya,&nbsp;Alexandros Charitos,&nbsp;Olena Volkova","doi":"10.1111/jace.20103","DOIUrl":"10.1111/jace.20103","url":null,"abstract":"<p>Oxide particles are considered to be one of the reasons for the stability of cellular porous Al foam. Thus, the contact angle (<i>ө</i>) of molten pure aluminum on oxide substrates, including Al<sub>2</sub>O<sub>3</sub>, CaO·2Al<sub>2</sub>O<sub>3</sub> (CA2), CaO·6Al<sub>2</sub>O<sub>3</sub> (CA6), mullite (3Al<sub>2</sub>O<sub>3</sub>·2SiO<sub>2</sub>), and SiO<sub>2</sub> was measured in a vacuum heating microscope at a temperature of 950°C to determine the value of wettability of molten aluminum on various oxides. Thereafter, the measured contact angles followed the tendency as mullite (155°) &gt; CA6 (152°) &gt; MgAl<sub>2</sub>O<sub>4</sub> (151°) &gt; Al<sub>2</sub>O<sub>3</sub> (149°) &gt; SiO<sub>2</sub> (124°) &gt; CA2 (100°). Furthermore, the cross-sectional area between molten aluminum and substrates was thoroughly analyzed, and the reaction products, such as the Al<sub>2</sub>O<sub>3</sub> layer at the interface, have been detected. Thermo-Calc, with the combination of available databases, was used to perform thermodynamic simulations and to discuss and predict possible reactions under the current experimental conditions.</p>","PeriodicalId":200,"journal":{"name":"Journal of the American Ceramic Society","volume":"108 1","pages":""},"PeriodicalIF":3.5,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1111/jace.20103","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142198254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic effects on dielectric and complex impedance properties in Ti3AlC2 MAX phase-infused PVDF-HFP/PMMA nanocomposites Ti3AlC2 MAX 相注入 PVDF-HFP/PMMA 纳米复合材料的介电性能和复合阻抗性能的协同效应
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-08-27 DOI: 10.1111/jace.20066
Subhasree Panda, S. K. Khadheer Pasha

A simple solution casting technique was used to formulate films of polyvinylidenefluoride-co-hexafluoropropylene, polymethylmethacrylate, and Ti3AlC2 MAX phase polymer nanocomposites (PPT) with different filler content. The functional groups present in the PPT films were studied using the Fourier transform infrared spectroscopy and the nature of crystallinity was observed using X-ray diffraction technique. The morphology of the films was studied by scanning electron microscopy. The thermal analysis was done using the thermogravimetric analysis and differential thermogravimetry analysis. The tensile behavior of the prepared films was studied from the stress-strain graphs. The ultraviolet–visible spectra revealed their optical characteristics. The dielectric parameters of the polymer blend and nanocomposite films like dielectric constant, loss tangent, AC conductivity, and complex impedance spectroscopy with corresponding equivalent circuits were studied. A comparative study of the above parameters was done for both the polymer blend and nanocomposites to find out the advancement in the properties of the prepared nanocomposite compared with the polymer blend. The nanocomposite film having 3 wt% of Ti3AlC2 MAX phase filler loading exhibited the best properties among all the nanocomposites. The enhanced dielectric properties of the nanocomposites with mechanical and thermal resistance can be used for real-time efficient energy storage applications.

采用简单的溶液浇铸技术配制了不同填料含量的聚偏氟乙烯-六氟丙烯、聚甲基丙烯酸甲酯和 Ti3AlC2 MAX 相聚合物纳米复合材料(PPT)薄膜。使用傅里叶变换红外光谱法研究了 PPT 薄膜中存在的官能团,并使用 X 射线衍射技术观察了结晶的性质。用扫描电子显微镜研究了薄膜的形态。热分析采用热重分析和差热重分析法进行。通过应力-应变图研究了制备薄膜的拉伸行为。紫外-可见光谱显示了它们的光学特性。研究了聚合物共混物和纳米复合薄膜的介电参数,如介电常数、损耗正切、交流电导率、复阻抗光谱以及相应的等效电路。对聚合物混合物和纳米复合材料的上述参数进行了比较研究,以发现所制备的纳米复合材料与聚合物混合物相比在性能上的进步。在所有纳米复合材料中,Ti3AlC2 MAX 相填料含量为 3 wt% 的纳米复合薄膜表现出最佳性能。纳米复合材料的介电性能增强,同时具有机械和耐热性能,可用于实时高效储能应用。
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引用次数: 0
Macroporous high-entropy spinel oxide monoliths as efficient oxygen evolution electrocatalyst 作为高效氧进化电催化剂的大孔高熵尖晶石氧化物单片
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-08-26 DOI: 10.1111/jace.20098
Xin Ouyang, Zhizhen Zhang, Tengteng Qin, Zhen Pei, Xingzhong Guo

In this paper, macroporous high-entropy spinel oxide (HESO) (Fe0.2Ni0.2Co0.2Mn0.2Zn0.2)3O4 monoliths were successfully fabricated via a sol–gel method followed by calcination. Appropriate polyacrylic acid and propylene oxide contents allow the formation of three-dimensional co-continuous xerogel monoliths, and the water/glycerol ratio controls the macropore size of monoliths. Subsequent calcination achieves the precipitation of HESO (Fe0.2Ni0.2Co0.2Mn0.2Zn0.2)3O4 with a singular phase and exceptional structural stability. The macroporous HESO (Fe0.2Ni0.2Co0.2Mn0.2Zn0.2)3O4 demonstrates remarkable performance in the oxygen evolution reaction (OER) with an overpotential of 333 mV at 100 mA cm−2 and a Tafel slope of 43.2 mV dec–1, surpassing that of RuO2 (391 mV) under identical conditions. Furthermore, the catalytic stability of the HESO catalyst remains superior even after 24 h of testing. This process offers a promising avenue for the development of macroporous high-entropy oxide OER catalysts for overall water splitting.

本文通过溶胶-凝胶法和煅烧法成功制备了大孔高熵尖晶石氧化物(HESO)(Fe0.2Ni0.2Co0.2Mn0.2Zn0.2)3O4单片。适当的聚丙烯酸和环氧丙烷含量可以形成三维共连续的异凝胶单体,而水/甘油的比例则控制着单体的大孔尺寸。随后的煅烧实现了 HESO(Fe0.2Ni0.2Co0.2Mn0.2Zn0.2)3O4 的沉淀,这种沉淀具有单相和优异的结构稳定性。大孔 HESO(Fe0.2Ni0.2Co0.2Mn0.2Zn0.2)3O4 在氧进化反应(OER)中表现出卓越的性能,在 100 mA cm-2 条件下过电位为 333 mV,Tafel 斜率为 43.2 mV dec-1,超过了相同条件下的 RuO2(391 mV)。此外,即使经过 24 小时的测试,HESO 催化剂的催化稳定性仍然非常出色。该工艺为开发用于整体水分离的大孔高熵氧化物 OER 催化剂提供了一条前景广阔的途径。
{"title":"Macroporous high-entropy spinel oxide monoliths as efficient oxygen evolution electrocatalyst","authors":"Xin Ouyang,&nbsp;Zhizhen Zhang,&nbsp;Tengteng Qin,&nbsp;Zhen Pei,&nbsp;Xingzhong Guo","doi":"10.1111/jace.20098","DOIUrl":"10.1111/jace.20098","url":null,"abstract":"<p>In this paper, macroporous high-entropy spinel oxide (HESO) (Fe<sub>0.2</sub>Ni<sub>0.2</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>Zn<sub>0.2</sub>)<sub>3</sub>O<sub>4</sub> monoliths were successfully fabricated via a sol–gel method followed by calcination. Appropriate polyacrylic acid and propylene oxide contents allow the formation of three-dimensional co-continuous xerogel monoliths, and the water/glycerol ratio controls the macropore size of monoliths. Subsequent calcination achieves the precipitation of HESO (Fe<sub>0.2</sub>Ni<sub>0.2</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>Zn<sub>0.2</sub>)<sub>3</sub>O<sub>4</sub> with a singular phase and exceptional structural stability. The macroporous HESO (Fe<sub>0.2</sub>Ni<sub>0.2</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>Zn<sub>0.2</sub>)<sub>3</sub>O<sub>4</sub> demonstrates remarkable performance in the oxygen evolution reaction (OER) with an overpotential of 333 mV at 100 mA cm<sup>−2</sup> and a Tafel slope of 43.2 mV dec<sup>–1</sup>, surpassing that of RuO<sub>2</sub> (391 mV) under identical conditions. Furthermore, the catalytic stability of the HESO catalyst remains superior even after 24 h of testing. This process offers a promising avenue for the development of macroporous high-entropy oxide OER catalysts for overall water splitting.</p>","PeriodicalId":200,"journal":{"name":"Journal of the American Ceramic Society","volume":"107 12","pages":"8354-8366"},"PeriodicalIF":3.5,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142198255","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Structural properties, dielectric relaxation, and impedance spectroscopy of NASICON type Na 3 + x Zr 2 − x Pr x Si 2 PO 12 ${rm Na}_{3+x} {rm Zr}_{2-x} {rm Pr}_{x} {rm Si}_2 {rm PO}_{12}$ ceramics NASICON 型 Na3+xZr2-xPrxSi2PO12 陶瓷的结构特性、介电常数弛豫和阻抗谱分析
IF 3.5 3区 材料科学 Q1 MATERIALS SCIENCE, CERAMICS Pub Date : 2024-08-26 DOI: 10.1111/jace.20101
Ramcharan Meena, Rajendra S. Dhaka
<p>We investigate the dielectric and impedance spectroscopic investigation of Pr-doped NASICON type <span></span><math> <semantics> <mrow> <msub> <mi>Na</mi> <mrow> <mn>3</mn> <mo>+</mo> <mi>x</mi> </mrow> </msub> <msub> <mi>Zr</mi> <mrow> <mn>2</mn> <mo>−</mo> <mi>x</mi> </mrow> </msub> <msub> <mi>Pr</mi> <mi>x</mi> </msub> <msub> <mi>Si</mi> <mn>2</mn> </msub> <msub> <mi>PO</mi> <mn>12</mn> </msub> </mrow> <annotation>${rm Na}_{3+x} {rm Zr}_{2-x} {rm Pr}_{x} {rm Si}_2 {rm PO}_{12}$</annotation> </semantics></math> (<span></span><math> <semantics> <mrow> <mi>x</mi> <mo>=</mo> <mn>0.05</mn> <mo>−</mo> <mn>0.2</mn> </mrow> <annotation>$x = 0.05 - 0.2$</annotation> </semantics></math>) samples as a function of temperature and frequency. The Rietveld refinement of X-ray diffraction patterns confirms the monoclinic phase having <i>C</i>2/<i>c</i> space groups for all the samples. The scanning electron microscopy shows the granular-like structure and energy dispersive X-ray analysis confirms the desired compositions. The temperature (90–400 K) and frequency (20 Hz–2 MHz) dependence of electric permittivity are explained using Maxwell–Wagner–Sillars (MWS) polarization and space charge polarization mechanisms. The dielectric relaxation shows nearly equal activation energy for all the samples with a non-Debye type of relaxation in the measured temperature range. The complex impedance analysis shows the presence of broad grain and grain boundary relaxation peaks. The stretched exponent analysis of electric modulus using the Kohlrausch–Williams–Watts (KWW) function further confirms the non-Debye type of relaxation. Moreover, scaling analysis of the electric modulus shows a similar type of relaxation for all the samples. The ac conductivity data are fitted using modified power law, where the temperature dependence of exponent (<span></span><math> <semantics> <mi>s</mi> <annotation>$s$</annotation> </semantics></math>) confirms the correlated barrier hopping (CBH) type conduction for all the samples. Our results indicate that the Pr-doped NASICON samples are potential candidates for charge storage devices due to thei
我们对掺杂 Pr 的 NASICON 型 Na3+xZr2-xPrxSi2PO12${rm Na}_{3+x} 进行了介电和阻抗光谱研究。{rm Zr}_{2-x}{rm Pr}_{x}{rm Si}_2 {rm PO}_{12}$ (x=0.05-0.2$x = 0.05 - 0.2$)样品是温度和频率的函数。X 射线衍射图样的里特维尔德细化证实,所有样品都是具有 C2/c 空间群的单斜相。扫描电子显微镜显示了颗粒状结构,能量色散 X 射线分析证实了所需的成分。电导率与温度(90-400 K)和频率(20 Hz-2 MHz)的关系可通过 Maxwell-Wagner-Sillars (MWS) 极化和空间电荷极化机制来解释。介电弛豫显示,在测量温度范围内,所有样品的活化能几乎相等,都是非德拜型弛豫。复阻抗分析表明存在广泛的晶粒和晶界弛豫峰。使用 Kohlrausch-Williams-Watts(KWW)函数对电模量进行的拉伸指数分析进一步证实了非戴贝松弛类型。此外,电模量的缩放分析表明所有样品的弛豫类型相似。交流传导数据使用修正幂律进行拟合,其中指数(s$s$)的温度依赖性证实了所有样品的相关势垒跳变(CBH)型传导。我们的研究结果表明,掺镨的 NASICON 样品具有较大的电导率,因此有可能成为电荷存储设备的候选材料。
{"title":"Structural properties, dielectric relaxation, and impedance spectroscopy of NASICON type \u0000 \u0000 \u0000 \u0000 Na\u0000 \u0000 3\u0000 +\u0000 x\u0000 \u0000 \u0000 \u0000 Zr\u0000 \u0000 2\u0000 −\u0000 x\u0000 \u0000 \u0000 \u0000 Pr\u0000 x\u0000 \u0000 \u0000 Si\u0000 2\u0000 \u0000 \u0000 PO\u0000 12\u0000 \u0000 \u0000 ${rm Na}_{3+x} {rm Zr}_{2-x} {rm Pr}_{x} {rm Si}_2 {rm PO}_{12}$\u0000 ceramics","authors":"Ramcharan Meena,&nbsp;Rajendra S. Dhaka","doi":"10.1111/jace.20101","DOIUrl":"10.1111/jace.20101","url":null,"abstract":"&lt;p&gt;We investigate the dielectric and impedance spectroscopic investigation of Pr-doped NASICON type &lt;span&gt;&lt;/span&gt;&lt;math&gt;\u0000 &lt;semantics&gt;\u0000 &lt;mrow&gt;\u0000 &lt;msub&gt;\u0000 &lt;mi&gt;Na&lt;/mi&gt;\u0000 &lt;mrow&gt;\u0000 &lt;mn&gt;3&lt;/mn&gt;\u0000 &lt;mo&gt;+&lt;/mo&gt;\u0000 &lt;mi&gt;x&lt;/mi&gt;\u0000 &lt;/mrow&gt;\u0000 &lt;/msub&gt;\u0000 &lt;msub&gt;\u0000 &lt;mi&gt;Zr&lt;/mi&gt;\u0000 &lt;mrow&gt;\u0000 &lt;mn&gt;2&lt;/mn&gt;\u0000 &lt;mo&gt;−&lt;/mo&gt;\u0000 &lt;mi&gt;x&lt;/mi&gt;\u0000 &lt;/mrow&gt;\u0000 &lt;/msub&gt;\u0000 &lt;msub&gt;\u0000 &lt;mi&gt;Pr&lt;/mi&gt;\u0000 &lt;mi&gt;x&lt;/mi&gt;\u0000 &lt;/msub&gt;\u0000 &lt;msub&gt;\u0000 &lt;mi&gt;Si&lt;/mi&gt;\u0000 &lt;mn&gt;2&lt;/mn&gt;\u0000 &lt;/msub&gt;\u0000 &lt;msub&gt;\u0000 &lt;mi&gt;PO&lt;/mi&gt;\u0000 &lt;mn&gt;12&lt;/mn&gt;\u0000 &lt;/msub&gt;\u0000 &lt;/mrow&gt;\u0000 &lt;annotation&gt;${rm Na}_{3+x} {rm Zr}_{2-x} {rm Pr}_{x} {rm Si}_2 {rm PO}_{12}$&lt;/annotation&gt;\u0000 &lt;/semantics&gt;&lt;/math&gt; (&lt;span&gt;&lt;/span&gt;&lt;math&gt;\u0000 &lt;semantics&gt;\u0000 &lt;mrow&gt;\u0000 &lt;mi&gt;x&lt;/mi&gt;\u0000 &lt;mo&gt;=&lt;/mo&gt;\u0000 &lt;mn&gt;0.05&lt;/mn&gt;\u0000 &lt;mo&gt;−&lt;/mo&gt;\u0000 &lt;mn&gt;0.2&lt;/mn&gt;\u0000 &lt;/mrow&gt;\u0000 &lt;annotation&gt;$x = 0.05 - 0.2$&lt;/annotation&gt;\u0000 &lt;/semantics&gt;&lt;/math&gt;) samples as a function of temperature and frequency. The Rietveld refinement of X-ray diffraction patterns confirms the monoclinic phase having &lt;i&gt;C&lt;/i&gt;2/&lt;i&gt;c&lt;/i&gt; space groups for all the samples. The scanning electron microscopy shows the granular-like structure and energy dispersive X-ray analysis confirms the desired compositions. The temperature (90–400 K) and frequency (20 Hz–2 MHz) dependence of electric permittivity are explained using Maxwell–Wagner–Sillars (MWS) polarization and space charge polarization mechanisms. The dielectric relaxation shows nearly equal activation energy for all the samples with a non-Debye type of relaxation in the measured temperature range. The complex impedance analysis shows the presence of broad grain and grain boundary relaxation peaks. The stretched exponent analysis of electric modulus using the Kohlrausch–Williams–Watts (KWW) function further confirms the non-Debye type of relaxation. Moreover, scaling analysis of the electric modulus shows a similar type of relaxation for all the samples. The ac conductivity data are fitted using modified power law, where the temperature dependence of exponent (&lt;span&gt;&lt;/span&gt;&lt;math&gt;\u0000 &lt;semantics&gt;\u0000 &lt;mi&gt;s&lt;/mi&gt;\u0000 &lt;annotation&gt;$s$&lt;/annotation&gt;\u0000 &lt;/semantics&gt;&lt;/math&gt;) confirms the correlated barrier hopping (CBH) type conduction for all the samples. Our results indicate that the Pr-doped NASICON samples are potential candidates for charge storage devices due to thei","PeriodicalId":200,"journal":{"name":"Journal of the American Ceramic Society","volume":"107 12","pages":"8378-8395"},"PeriodicalIF":3.5,"publicationDate":"2024-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142198256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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Journal of the American Ceramic Society
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