Solid State Ionics最新文献_第2页

Research on synthesis process and calcination reaction mechanism of porous LLZO with high specific surface area 高比表面积多孔LLZO的合成工艺及煅烧反应机理研究

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-12-01 DOI: 10.1016/j.ssi.2025.117086

Shengdong Tao , Jian Li , Yali Liu , Zulv Huang , Hui Fu , Guowen He , Kun Shen , Zheng Liu , Zhifang Yin

Garnet-type Li₇La₃Zr₂O₁₂ (LLZO), a promising solid-state electrolyte due to its high ionic conductivity, wide electrochemical window, and stability against metallic lithium, has attracted significant attention in recent years. However, its practical application is severely limited by drawbacks, including insufficient mechanical flexibility, prolonged synthesis/calcination times and challenging process control. This study proposes a metal-organic framework (MOF)-mediated strategy for LLZO synthesis. Specifically, La-Zr-MOF was constructed via hydrothermal self-assembly in solution, leveraging the strong coordination of carboxylate ligands with La³⁺ and Zr⁴⁺ ions. Subsequent incorporation of a lithium salt yields an LLZO precursor with atomic-level homogeneous dispersion of La, Zr, and Li. Direct calcination of the precursor produced phase-pure LLZO in a single step. Through process optimization, employing polyethylene glycol-200 (PEG-200) as the MOF synthesis solvent, LiAc as the lithium source, and 20 mol% lithium excess, cubic-phase LLZO with a high specific surface area (144.76 m² g⁻¹) was successfully synthesized at a relatively low temperature (1000 °C) with a short holding time (5 h). Furthermore, the calcination mechanism of LLZO was elucidated by SEM, XRD, TEM, specific surface area analysis and pore size distribution analysis of samples calcined at different temperatures. This research provides a novel strategy for the low-temperature, rapid synthesis of high-surface-area cubic-phase LLZO.

石榴石型Li7La3Zr2O12 （LLZO）具有离子电导率高、电化学窗口宽、抗金属锂稳定性好等优点，近年来受到广泛关注。然而，它的实际应用受到一些缺点的严重限制，包括机械灵活性不足、合成/煅烧时间长和过程控制困难。本研究提出了一种金属有机框架（MOF）介导的LLZO合成策略。具体来说，利用羧酸配体与La3+和Zr4+离子的强配位，通过水热自组装在溶液中构建了La-Zr-MOF。随后加入锂盐产生具有原子水平均匀分散的La、Zr和Li的LLZO前驱体。前驱体直接煅烧一步制得相纯LLZO。通过工艺优化，以聚乙二醇-200 （PEG-200）为MOF合成溶剂，LiAc为锂源，过量锂量为20 mol%，在相对较低的温度（1000℃）和较短的保温时间（5 h）下成功合成了高比表面积（144.76 m2 g−1）的立方相LLZO。通过SEM、XRD、TEM、比表面积分析和不同温度下煅烧样品的孔径分布分析，阐明了LLZO的煅烧机理。本研究为低温、快速合成高比表面积的三相LLZO提供了一条新思路。

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引用次数: 0

Preparation of partially Y- or Yb-substituted SrFeO3-δ with cubic perovskite structure and its electrical conduction properties 立方钙钛矿结构部分Y或yb取代SrFeO3-δ的制备及其导电性能

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-11-21 DOI: 10.1016/j.ssi.2025.117073

Keina Nagai , Chihiro Kato , Ryutaro Maehara , Taizo Yoshino , Takayuki Sugimoto , Kosuke Shido , Takuya Hashimoto , Fumito Fujishiro , Eiki Niwa , Motoyuki Matsuo

SrFeO_3-δ prepared in air exhibits a tetragonal or orthorhombic perovskite crystal structure with an ordered distribution of oxide-ion vacancies at room temperature. Changing the crystal structure to cubic perovskite with a random distribution of oxide-ion vacancies is expected to improve the hole or oxide-ion conductivity. In this study, the crystal structure of SrFeO_3-δ was altered by partially substituting Y or Yb at the Sr or Fe sites. X-ray diffraction and X-ray absorption spectroscopy revealed that Y partially substituted only at the Sr site, whereas Yb could substitute at both the Sr and Fe sites. Both substitutions resulted in a cubic perovskite structure. Mössbauer spectroscopy detected charge delocalization from the Y- or Yb-substitution in the cubic phase. The degree of delocalization was higher in the Sr-site-substituted specimen than in the Fe-site-substituted specimen. The cubic phases of Sr_1-xY_xFeO_3-δ, Sr_1-xYb_xFeO_3-δ, and SrFe_1-xYb_xO_3-δ exhibited a semiconducting temperature dependence devoid of phase transition effects. The lower electrical conductivity of SrFe_1-xYb_xO_3-δ compared with that of Sr_1-xYb_xFeO_3-δ corresponded to the lower delocalization degree observed by Mössbauer spectroscopy. Sr_0.9Y_0.1FeO_3-δ and Sr_0.9Yb_0.1FeO_3-δ exhibited electrical conductivity comparable with that of cubic SrFeO_2.75 above 420 °C without the structural phase transition influence, indicating their application potential, e.g., for gas separation and electrodes in solid oxide fuel cells.

在空气中制备的SrFeO3-δ在室温下表现为四方或正交钙钛矿晶体结构，氧化离子空位分布有序。将晶体结构改变为具有随机分布的氧化离子空位的立方钙钛矿有望改善空穴或氧化离子的电导率。在本研究中，通过在Sr或Fe位点部分取代Y或Yb，改变了SrFeO3-δ的晶体结构。x射线衍射和x射线吸收光谱显示，Y仅部分取代Sr位，而Yb可以取代Sr位和Fe位。这两种取代都产生了立方钙钛矿结构。Mössbauer光谱检测到立方相中Y-或Y-取代的电荷离域。sr -取代样品的离域程度高于fe -取代样品。Sr1-xYxFeO3-δ、Sr1-xYbxFeO3-δ和SrFe1-xYbxO3-δ的立方相表现出半导体温度依赖性，没有相变效应。与sr1 - xybxo3 -δ相比，srfe1 - xybxfeo3 -δ的电导率较低，这与Mössbauer光谱观察到的较低的离域程度相对应。Sr0.9Y0.1FeO3-δ和Sr0.9Yb0.1FeO3-δ在420°C以上表现出与立方SrFeO2.75相当的电导率，而不受结构相变的影响，表明它们的应用潜力，例如用于气体分离和固体氧化物燃料电池的电极。

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引用次数: 0

Insights into ion transport in polymer electrolytes: Classifications, models and mechanisms 聚合物电解质中离子传输的见解：分类、模型和机制

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-11-19 DOI: 10.1016/j.ssi.2025.117083

Maitri Patel , Kuldeep Mishra , J.J. Chaudhari , Vaishali Madhani , Jehova Jire L. Hmar , Ashwani Kumar , Neeladri Das , Deepak Kumar

Polymer-based electrolytes have emerged as the most viable component for various electrochemical applications, including batteries, fuel cells, and supercapacitors, due to their unique combination of properties, such as competitive ionic conductivity, a high electrochemical stability window, and superior adhesion at the electrolyte/electrode interface with mechanical flexibility. To obtain the most suitable electrolyte system, these electrolyte systems have undergone through various structural and compositional modifications. There are different classes of polymer electrolytes. Understanding the ion-transport mechanisms in these complex materials is essential for optimizing their performance. This study offers a thorough examination of several models suggested for ion conduction in polymer electrolytes. The classical approaches, such as the vehicular and segmental motion models, as well as more recent theories, including the Vogel-Tammann-Fulcher (VTF) model, dynamic bond percolation, and hopping mechanisms, are discussed in detail. Emphasis is given to the interplay between polymer segmental motion and ion transport, the role of ion–polymer interactions, the role of different fillers and plasticizers, and the influence of structural heterogeneity on conduction pathways. This work also highlights the strengths and limitations of the ion conduction models.

聚合物电解质已成为各种电化学应用中最可行的组件，包括电池、燃料电池和超级电容器，因为它们具有独特的组合特性，如竞争性离子电导率、高电化学稳定性窗口以及在电解质/电极界面具有机械灵活性的优越附着性。为了获得最合适的电解质体系，这些电解质体系经过了各种结构和成分的修饰。聚合物电解质有不同的种类。了解这些复杂材料中的离子传输机制对于优化其性能至关重要。本研究对聚合物电解质中离子传导的几种模型进行了全面的研究。经典的方法，如车辆和节段运动模型，以及最近的理论，包括Vogel-Tammann-Fulcher （VTF）模型，动态键渗透和跳跃机制，进行了详细的讨论。重点是聚合物节段运动与离子传递之间的相互作用，离子-聚合物相互作用的作用，不同填料和增塑剂的作用，以及结构不均匀性对传导途径的影响。这项工作也突出了离子传导模型的优势和局限性。

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引用次数: 0

Bi-material cathodes based on O3-type NaNi1/3Fe1/3Mn1/3O2 and activated carbon for high-energy hybrid sodium ion battery capacitors 基于o3型NaNi1/3Fe1/3Mn1/3O2和活性炭的高能混合钠离子电池电容器双材料阴极

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-11-18 DOI: 10.1016/j.ssi.2025.117071

Hengheng Xia , Chongyang Yang , Zhongxun An , Yue-Ling Bai , Jiaqiang Xu

Hybrid sodium ion battery capacitor (SIBC) is a type of internal hybrid electrochemical energy storage device featuring a dual-energy storage mechanism, capable of delivering high energy and power densities. In this work, we have developed high-energy SIBCs using bi-material cathodes composed of NaNi_1/3Fe_1/3Mn_1/3O₂ (NFM) and activated carbon (AC), paired with presodiation-free hard carbon anodes. NFM offers high capacity but suffers from poor conductivity and rate capability, whereas AC enhances kinetics but limits energy density. Through optimization of the AC/NFM mass ratio in commercial-scale pouch-type full cells, we demonstrate that a hybrid cathode with 9.1 wt% AC (R_1/10) achieves optimal electrochemical performance. This design effectively balances battery-type (NFM) and capacitor-type (AC) materials, resulting in a significant reduction in electrode resistance from 19.4 mΩ to 10.8 mΩ, along with decreased interfacial film resistance and charge transfer resistance, thereby enhancing capacitive contribution. The R_1/10 SIBC delivers a high energy density of 161.3 Wh kg⁻¹ at 74.8 W kg⁻¹ and maintains 62.3 Wh kg⁻¹ at 11.8 kW kg⁻¹, outperforming pure NFM cells. It also exhibits enhanced low-temperature performance with 38.0 % capacity retention at −20 °C (5C), superior cycling stability with 72.2 % capacity retention after 10,000 cycles at 10C, and minimal self-discharge at 60 °C (0.5 mV h⁻¹). The synergy between AC and NFM mitigates polarization, accelerates reaction kinetics, and broadens the practical applicability of high-power energy storage systems.

混合钠离子电池电容器（SIBC）是一种具有双能量存储机制的内部混合电化学储能装置，能够提供高能量密度和功率密度。在这项工作中，我们开发了高能SIBCs，使用由NaNi1/3Fe1/3Mn1/3O2 （NFM）和活性炭（AC）组成的双材料阴极，搭配无预沉淀的硬碳阳极。NFM提供高容量，但电导率和速率能力差，而交流电提高了动力学，但限制了能量密度。通过优化商业规模的袋式全电池中AC/NFM的质量比，我们证明了9.1 wt% AC （R1/10）的混合阴极获得了最佳的电化学性能。这种设计有效地平衡了电池型（NFM）和电容器型（AC）材料，使电极电阻从19.4 mΩ显著降低到10.8 mΩ，同时降低了界面膜电阻和电荷转移电阻，从而提高了电容的贡献。R1/10 SIBC在74.8 W kg - 1时提供161.3 Wh kg - 1的高能量密度，在11.8 kW kg - 1时保持62.3 Wh kg - 1，优于纯NFM电池。它还表现出增强的低温性能，在- 20°C （5C）下容量保持率为38.0%，在10°C下循环10000次后容量保持率为72.2%，在60°C （0.5 mV h - 1）下自放电最小。AC和NFM之间的协同作用减轻了极化，加速了反应动力学，拓宽了大功率储能系统的实际适用性。

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引用次数: 0

Novel oxygen-ion conductors Ln10W22O81 (Ln = La, Ce, Pr, Nd) 新型氧离子导体Ln10W22O81 （Ln = La, Ce, Pr, Nd）

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-11-15 DOI: 10.1016/j.ssi.2025.117072

A. Guseva, N. Pestereva, V. Gardt, D. Kuznetsov

Lanthanide tungstates Ln₁₀W₂₂O₈₁ (Ln = La, Ce, Pr, Nd) were prepared by the by solid-state reaction technique and their electrical conductivity have been examined by the electrochemical impedance method. Predominant ionic conductivity in Ln₁₀W₂₂O₈₁ (Ln = La, Pr, Nd) was established both by the EMF method and from independence of conductivity versus oxygen partial pressure. Ce₁₀W₂₂O₈₁ reveals some contribution of the electronic p-type component. The Tubandt method established that the ionic charge carriers in lanthanide tungstates are oxygen ions. It was found that the electrical conductivity of the studied lanthanide tungstates decreases in the order Ce₁₀W₂₂O_81, Pr₁₀W₂₂O₈₁, La₁₀W₂₂O₈₁, Nd₁₀W₂₂O₈₁. Of all the compounds studied, praseodymium tungstate has the highest oxygen-ion conductivity (3.2 × 10⁻⁴ S/cm at 800 °C), which makes it the most promising for further research and application in solid-state ionics.

采用固相反应法制备了镧系钨酸盐Ln10W22O81 (Ln = La, Ce, Pr, Nd)，并用电化学阻抗法对其电导率进行了测试。通过电动势法和电导率与氧分压的独立关系，确定了Ln10W22O81的主要离子电导率（Ln = La, Pr, Nd）。Ce10W22O81显示了电子p型元件的一些贡献。Tubandt方法确定了镧系钨酸盐中的离子载流子是氧离子。结果表明，镧系钨酸盐的电导率依次为Ce10W22O81、Pr10W22O81、La10W22O81、Nd10W22O81。在所研究的化合物中，钨酸镨具有最高的氧离子电导率（在800°C时为3.2 × 10−4 S/cm），这使其在固态离子中具有进一步研究和应用的前景。

{"title":"Novel oxygen-ion conductors Ln10W22O81 (Ln = La, Ce, Pr, Nd)","authors":"A. Guseva, N. Pestereva, V. Gardt, D. Kuznetsov","doi":"10.1016/j.ssi.2025.117072","DOIUrl":"10.1016/j.ssi.2025.117072","url":null,"abstract":"<div><div>Lanthanide tungstates Ln10W22O81 (Ln = La, Ce, Pr, Nd) were prepared by the by solid-state reaction technique and their electrical conductivity have been examined by the electrochemical impedance method. Predominant ionic conductivity in Ln10W22O81 (Ln = La, Pr, Nd) was established both by the EMF method and from independence of conductivity versus oxygen partial pressure. Ce10W22O81 reveals some contribution of the electronic p-type component. The Tubandt method established that the ionic charge carriers in lanthanide tungstates are oxygen ions. It was found that the electrical conductivity of the studied lanthanide tungstates decreases in the order Ce10W22O81, Pr10W22O81, La10W22O81, Nd10W22O81. Of all the compounds studied, praseodymium tungstate has the highest oxygen-ion conductivity (3.2 × 10−4 S/cm at 800 °C), which makes it the most promising for further research and application in solid-state ionics.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"433 ","pages":"Article 117072"},"PeriodicalIF":3.3,"publicationDate":"2025-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145527943","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

Polycarbonate-based polymer electrolytes for potassium batteries 钾电池用聚碳酸酯基聚合物电解质

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-11-12 DOI: 10.1016/j.ssi.2025.117069

Isabell Lee Johansson , Timofey I. Kolesnikov , Anna Khudyshkina , Ulf-Christian Rauska , Daniel Brandell , Jonas Mindemark , Guiomar Hernández , Fabian Jeschull

Polycarbonate-based solid polymer electrolytes (SPEs) are being intensively studied for use in all-solid-state batteries as a viable alternative to the commonly used poly(ethylene oxide)-based SPEs. Specifically, poly(trimethylene carbonate) (PTMC) and poly(ε-caprolactone–co–trimethylene carbonate) (P(CL-TMC)) as a well-performing copolymeric derivative represent two materials classes that so far have not been studied in potassium battery applications. Herein, we aim to close this knowledge gap by studying physical material properties of PTMC and P(CL-TMC) solid electrolytes with potassium bis(trifluoromethanesulfonyl)imide (KTFSI) as conductive salt and examine their electrochemical stability and characteristics in K-metal/K₂Fe[Fe(CN)₆] (KFF), as well as Fe[Fe(CN)₆/K₂Fe[Fe(CN)₆] cell configurations. While operation of polycarbonate-based solid-state potassium batteries at temperatures as low as 40 °C is feasible, comparatively low discharge capacities and capacity retention were observed in comparison to polyether-based systems. For the P(CL-TMC) material, rapid degradation through depolymerization processes in direct contact with potassium metal represents a major bottleneck. With this study, we set a starting point for further materials development in alternative polymer hosts for SPE applications in potassium batteries.

聚碳酸酯基固体聚合物电解质（spe）正被广泛研究用于全固态电池，作为常用的聚环氧乙烷基spe的可行替代品。具体来说，聚（三亚甲基碳酸酯）（PTMC）和聚（ε-己内酯-共三亚甲基碳酸酯）（P(CL-TMC)）作为一种性能良好的共聚衍生物，代表了迄今尚未在钾电池应用中研究的两类材料。本文旨在通过研究以二（三氟甲烷磺酰）亚胺钾（KTFSI）为导电盐的PTMC和P（CL-TMC）固体电解质的物理材料性质，以及它们在K-metal/K2Fe[Fe(CN)6] （KFF）和Fe[Fe(CN)6] /K2Fe[Fe(CN)6]电池构型中的电化学稳定性和特性，来弥补这一知识空白。虽然聚碳酸酯基固态钾电池在低至40°C的温度下运行是可行的，但与聚醚基电池相比，其放电容量和容量保持率相对较低。对于P（CL-TMC）材料来说，通过与金属钾直接接触的解聚过程进行快速降解是一个主要瓶颈。通过这项研究，我们为进一步开发用于钾电池中SPE应用的替代聚合物宿主材料奠定了起点。

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引用次数: 0

Electrical properties and conductivity mechanism for Ca2KH7(PO4)4·2H2O and Ca2(NH4)H7(PO4)4·2H2O Ca2KH7(PO4)4·2H2O和Ca2(NH4)H7(PO4)4·2H2O的电学性质及导电机理

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-11-10 DOI: 10.1016/j.ssi.2025.117070

K. Najkov , V. Koleva , V. Stefov , M. Pecovska Gjorgjevich

For the first time the acid salts Ca₂KH₇(PO₄)₄·2H₂O and Ca₂(NH₄)H₇(PO₄)₄·2H₂O are studied as potential proton conductors by complex impedance spectroscopy. Their electrical and dielectric properties, as well as conductivity are examined as a function of frequency (10 Hz–10 MHz) at various temperatures (293 K–363 K). The complex impedance spectra showed semicircle arcs depending on temperature indicating conductivity through grain boundaries with semiconducting behavior. It was found that for the two salts in the investigated temperature range the ac conductivity follows Joncher's power law and dc conductivity follows the Arrhenius behavior with activation energy 0.552 eV for Ca₂KH₇(PO₄)₄·2H₂O and 0.713 eV for Ca₂(NH₄)H₇(PO₄)₄·2H₂O. The results were confirmed with electric modulus analysis. The conductivity mechanism of the two compounds was also investigated and the experimental results were analyzed using various theoretical models. It has been established that the overlapping large polaron tunneling (OLPT) was the best model to explain the proton conduction of both acidic salts. Comparison of the conductivity with other phosphate proton conductors was made.

首次利用复阻抗谱技术研究了酸性盐Ca2KH7(PO4)4·2H2O和Ca2(NH4)H7(PO4)4·2H2O作为质子电位导体。在不同温度（293 K - 363 K）下，它们的电学和介电性能以及电导率作为频率（10 Hz-10 MHz）的函数进行了测试。复合阻抗谱随温度变化呈半圆弧，表明具有半导体行为的晶界电导率。结果表明，在研究温度范围内，两种盐的交流电导率服从Joncher幂定律，直流电导率服从Arrhenius行为，Ca2KH7(PO4)4·2H2O的活化能为0.552 eV, Ca2(NH4)H7(PO4)4·2H2O的活化能为0.713 eV。电模量分析证实了这一结果。研究了两种化合物的导电机理，并用各种理论模型对实验结果进行了分析。已经确定重叠大极化子隧穿（OLPT）是解释两种酸性盐的质子传导的最佳模型。并与其它磷酸盐质子导体的电导率进行了比较。

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引用次数: 0

Structural effects on oxygen vacancies and redox behavior in Mn-based perovskite oxides mn基钙钛矿氧化物中氧空位和氧化还原行为的结构影响

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-10-30 DOI: 10.1016/j.ssi.2025.117067

Vika Arzumanyan , Cijie Liu , Dawei Zhang , Wei Li , Jian Luo , Xingbo Liu , Yue Qi

A series of perovskite oxides

({Ln}_{2 / 3} A_{1 / 3}) Mn O_{3}

(Ln = La, Pr, Nd, Gd; A = Ba, Sr) was investigated to understand the effects of A-site cation size on oxygen vacancy formation. Quasirandom

(L n_{2 / 3} A_{1 / 3}) Mn O_{3}

mixed structures were generated using Alloy Theoretic Automated Toolkit (ATAT), followed by density functional theory (DFT) calculations. While mixing the orthorhombic

LnMn O_{3}

structures with the hexagonal AMnO₃ structures leads to lattices and global symmetries closer to cubic, the average volume generally increases with the average ionic size, and the local bond and angles exhibit more variations due to A-site mixing. DFT calculations and a statistical model were combined to predict oxygen reduction abilities. Thermogravimetric analysis (TGA) provided experimental validation of these predictions by measuring changes in oxygen non-stoichiometry (

Δδ

) under controlled conditions. Both indicated that larger A-site ionic size differences lead to greater

Δδ

, consistent with the larger variation in local structures, and enhanced redox capabilities. This combined computational-experimental approach highlights the importance of local structure variation, instead of average properties, in A-site cation engineering to optimize perovskite oxides for different devices relying on oxygen vacancy redox activity.

研究了一系列钙钛矿氧化物Ln2/3A1/3MnO3 (Ln = La, Pr, Nd, Gd; A = Ba, Sr)，以了解A位阳离子大小对氧空位形成的影响。利用Alloy theory Automated Toolkit （ATAT）生成准随机Ln2/3A1/3MnO3混合结构，并进行密度泛函理论（DFT）计算。当正交结构的LnMnO3与六方结构的AMnO3混合时，晶格和全局对称性更接近立方，平均体积一般随着平均离子尺寸的增加而增加，局域键和角度由于a位混合而表现出更多的变化。DFT计算和统计模型相结合来预测氧还原能力。热重分析（TGA）通过在受控条件下测量氧非化学计量学（Δδ）的变化，为这些预测提供了实验验证。两者都表明，较大的a位离子大小差异导致较大的Δδ，与较大的局部结构变化一致，并且增强了氧化还原能力。这种计算与实验相结合的方法强调了局部结构变化的重要性，而不是平均性质，在a位阳离子工程中，依靠氧空位氧化还原活性来优化不同器件的钙钛矿氧化物。

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引用次数: 0

Current and deformation in the single Li[Ni0.885 Co0.1 Al0.015]O2 nanoparticle studied by phase field simulation 用相场模拟方法研究了Li[Ni0.885 Co0.1 Al0.015]O2纳米颗粒中的电流和变形

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-10-30 DOI: 10.1016/j.ssi.2025.117047

Peng Dong , Jing Luo , Zhe Zhu , Xiangzhi Zeng

Understanding the electrochemical and mechanical behavior of single cathode particles is essential for advancing lithium-ion battery performance. This study combines nanoscale characterization and computational modeling to investigate the voltage-dependent responses of Li[Ni_0.885Co_0.1Al_0.015]O₂ (NCA) particles. Experimental measurements using conductive atomic force microscopy (CAFM) and electrochemical strain microscopy (ESM) under varying voltages were supported by a reconstructed two-dimensional realistic particle and an electrochemical-mechanical coupled model with anisotropic diffusion. Simulation results revealed that higher applied voltages increase the chemical potential for Li⁺ diffusion, enhancing ion transport and current response in CAFM, while stress gradients between the core and surface of particles lead to significant deformation observed in ESM. This work demonstrates the critical role of local electro-chemo-mechanical coupling in single-particle behavior and provides a microstructure-based interpretation of nanoscale phenomena.

了解单阴极颗粒的电化学和力学行为对提高锂离子电池的性能至关重要。本研究结合纳米尺度表征和计算模型研究Li[Ni0.885Co0.1Al0.015]O2 （NCA）粒子的电压依赖性响应。利用导电原子力显微镜（CAFM）和电化学应变显微镜（ESM）在不同电压下进行的实验测量得到了二维真实粒子重构和具有各向异性扩散的电化学-力学耦合模型的支持。模拟结果表明，较高的施加电压增加了Li+扩散的化学势，增强了CAFM中的离子传输和电流响应，而颗粒核心和表面之间的应力梯度导致ESM中观察到明显的变形。这项工作证明了局部电化学-机械耦合在单粒子行为中的关键作用，并提供了基于微观结构的纳米级现象的解释。

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引用次数: 0

Materials discovery through interpretation: An application to proton-conducting oxides 通过解释发现材料：在质子导电氧化物中的应用

IF 3.3 4区材料科学 Q3 CHEMISTRY, PHYSICAL

Solid State Ionics

Pub Date : 2025-10-27 DOI: 10.1016/j.ssi.2025.117054

Yoshihiro Yamazaki , Kota Tsujikawa , Junji Hyodo , Susumu Fujii

Machine learning has become a pivotal tool in materials discovery, but conventional data-driven models often behave as “black boxes” limited by the scope of their training data. In this perspective, we outline the current status of machine learning-driven materials discovery and present Materials Discovery through Interpretation (MDI), a framework that integrates scientific reasoning into the ML loop to enhance the reliability and impact of materials design. Instead of relying solely on statistical correlations, the MDI iteratively incorporates domain knowledge and insights from experimental and/or computational results such as phase formability and materials functionality into the predictive process. This interpretive strategy enables meaningful extrapolation even when underlying physics and chemical correlations remain poorly understood, guiding the identification of new candidate materials while simultaneously refining the models. Applied to proton-conducting oxides, MDI successfully identified previously unrecognized compounds, including those achieving conductivity above 0.01 Scm⁻¹ at 300 °C, a critical benchmark for fuel cell electrolytes, while providing clear rationales for their selection. By combining predictive power with interpretability, MDI offers a flexible pathway for accelerating materials innovation beyond the confines of existing data.

机器学习已经成为材料发现的关键工具，但传统的数据驱动模型往往表现得像“黑匣子”，受到其训练数据范围的限制。从这个角度来看，我们概述了机器学习驱动的材料发现的现状，并提出了通过解释发现材料（MDI），这是一个将科学推理集成到ML循环中的框架，以提高材料设计的可靠性和影响。MDI不再仅仅依赖于统计相关性，而是迭代地将领域知识和来自实验和/或计算结果的见解（如相成形性和材料功能）纳入预测过程。这种解释策略使得有意义的外推，即使在潜在的物理和化学相关性仍然知之甚少的情况下，指导新的候选材料的识别，同时改进模型。应用于质子导电氧化物，MDI成功识别了以前未被识别的化合物，包括那些在300°C（燃料电池电解质的关键基准）下电导率高于0.01 Scm−1的化合物，同时为它们的选择提供了明确的依据。通过将预测能力与可解释性相结合，MDI为加速材料创新提供了一种超越现有数据限制的灵活途径。

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引用次数: 0