Materials Today最新文献_第2页

Optimizing oxygen evolution/reduction reaction processes via anion vacancy engineering 通过阴离子空位工程优化析氧/还原反应过程

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.018

Wei Li , Da Liu , Ding Yuan , Porun Liu , Huakun Liu , Shixue Dou , Renbing Wu , Yuhai Dou

The increasing global energy demand and environmental challenges have highlighted the need for efficient, sustainable energy conversion technologies, particularly those involving the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). These reactions are crucial for electrochemical devices like water splitting, fuel cells and metal-air batteries, but their high overpotentials and energy requirements limit widespread application. Noble metal catalysts, though effective, are costly and scarce, prompting interest in transition metal alternatives. Anion vacancy engineering has shown promise in enhancing these catalysts’ performance. This review covers recent advancements in anion vacancy engineering for OER and ORR electrocatalysis, discussing fundamental mechanisms, strategies for creating anion vacancies (e.g., solution etching, plasma treatment), advanced characterization techniques (e.g., EPR, PAS, XPS), and how anion vacancies enhance catalytic performance through optimizing intermediate adsorption/desorption, improving metal-support interactions, facilitating catalyst reconstruction and so on. Challenges remain in precisely controlling anion vacancy synthesis, scaling up production, and understanding real-time structural changes in vacancy-rich catalysts. Future research should focus on novel synthesis techniques, in situ characterization methods, and leveraging machine learning to optimize these catalysts. This review aims to guide the development of efficient, sustainable energy conversion technologies using vacancy-engineered electrocatalysts.

日益增长的全球能源需求和环境挑战凸显了对高效、可持续的能源转换技术的需求，特别是涉及析氧反应（OER）和氧还原反应（ORR）的技术。这些反应对于水分解、燃料电池和金属-空气电池等电化学设备至关重要，但它们的高过电位和能量需求限制了它们的广泛应用。贵金属催化剂虽然有效，但价格昂贵且稀缺，这促使人们对过渡金属替代品产生了兴趣。阴离子空位工程在提高这些催化剂的性能方面显示出了希望。本文综述了OER和ORR电催化阴离子空位工程的最新进展，讨论了基本机制、产生阴离子空位的策略（如溶液蚀刻、等离子体处理）、先进的表征技术（如EPR、PAS、XPS），以及阴离子空位如何通过优化中间体吸附/解吸、改善金属-载体相互作用、促进催化剂重构等来提高催化性能。挑战仍然存在于精确控制阴离子空位合成、扩大生产和了解富空位催化剂的实时结构变化。未来的研究应该集中在新的合成技术、原位表征方法以及利用机器学习来优化这些催化剂上。本文综述旨在指导利用空位工程电催化剂开发高效、可持续的能源转换技术。

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引用次数: 0

Boosting internal quantum efficiency to near-unity in Fe3+-doped NIR phosphors: Structural engineering and energy transfer in A2LuSbO6 (A = Ba/Sr/Ca) double perovskites 将Fe3+掺杂近红外荧光粉的内部量子效率提高到接近统一：A2LuSbO6 （A = Ba/Sr/Ca）双钙钛矿的结构工程和能量转移

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.012

Haiping Luo , Shenglan Zhou , Wenjie Deng , Jiahao Liu , Jiaqing Peng , Bo Li , Zhihua Xiong , Wei Wang , Xinyu Ye

Fe³⁺ is a promising near-infrared (NIR) activator ion due to its tunable emission and non-toxicity, which has attracted growing interest. However, developing high-performance broadband NIR-emitting phosphors based on Fe³⁺ remains a significant challenge. In this work, we present Fe³⁺-activated A₂LuSbO₆ (A = Ba/Sr/Ca) double perovskite phosphors, which exhibit unusually long-wavelength NIR emission (>850 nm). By adopting a cation substitution strategy at the A-site, we designed the gradual replacement of large-radius ions with small-radius ions, achieving controllable tuning of emission from 847 nm to 937 nm. This substitution process simultaneously reduces structural symmetry and induces octahedral distortion, which breaks the spin-forbidden transition of Fe³⁺ and enhances luminescence performance. However, the continuous emission redshift leads to a large Stokes shift, which suppresses Fe³⁺ luminescence. The combined effect of these two factors results in optimal luminescence efficiency in Sr₂LuSbO₆:1.0 %Fe³⁺ (SLSO) sample, with internal/external quantum efficiencies (IQE/EQE) of 94.8 %/54.5 %. To further enhance luminescence performance, we introduced the rare-earth Yb³⁺, establishing an efficient Fe³⁺→Yb³⁺ energy transfer (ET) channel that reduces non-radiative transition losses. Compared with the Yb³⁺-free sample, the SLSO:1.0 %Fe³⁺, 3.0 %Yb³⁺ sample exhibits a broadened FWHM from 115 nm to 180 nm, enhanced IQE and EQE of 98.1 % and 56.4 %, respectively, and 13 % improved thermal stability. Finally, a pc-LED device based on the SLSO:1.0 %Fe³⁺, 3.0 %Yb³⁺ phosphor demonstrates potential for applications in NIR spectroscopy analysis, night vision, biomedical imaging, and other fields. This work lays a foundation for further research on strategies to regulation the optical properties of Fe³⁺-activated NIR phosphors.

Fe3+由于其发射可调和无毒性，是一种很有前途的近红外（NIR）激活离子，引起了人们越来越多的关注。然而，开发基于Fe3+的高性能宽带nir发光荧光粉仍然是一个重大挑战。在这项工作中，我们提出了Fe3+活化的A2LuSbO6 （A = Ba/Sr/Ca）双钙钛矿荧光粉，它表现出异常的长波近红外发射（>850 nm）。通过在a位采用阳离子取代策略，我们设计了大半径离子逐渐被小半径离子取代，实现了从847 nm到937 nm的可控调谐。这种取代过程同时降低了结构的对称性，引起了八面体畸变，打破了Fe3+的自旋禁止跃迁，提高了发光性能。然而，连续的发射红移导致了较大的Stokes位移，抑制了Fe3+的发光。在sr2lusbo6: 1.0% Fe3+ (SLSO)样品中，这两个因素的综合作用使其发光效率达到最佳，其内部/外部量子效率（IQE/EQE）为94.8% / 54.5%。为了进一步提高发光性能，我们引入了稀土Yb3+，建立了一个高效的Fe3+→Yb3+能量转移（ET）通道，减少了非辐射跃迁损失。与不含Yb3+的样品相比，SLSO: 1.0% Fe3+， 3.0% Yb3+样品的FWHM从115 nm扩大到180 nm， IQE和EQE分别提高了98.1%和56.4%，热稳定性提高了13%。最后，基于SLSO: 1.0% Fe3+， 3.0% Yb3+荧光粉的pc-LED器件展示了在近红外光谱分析，夜视，生物医学成像等领域的应用潜力。本研究为进一步研究Fe3+活化近红外荧光粉的光学特性调控策略奠定了基础。

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引用次数: 0

Honey-inspired thermally hysteretic adhesives for high strength and reversible underwater adhesion 受蜂蜜启发的热滞粘合剂，用于高强度和可逆的水下粘合

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.013

Xinlong Li , Wanshan Gao , Hao Zheng , Zhiyun Dong , Xiaoyu Huang , Hanjiao Chen , Hong Chen , Jiaojiao Yang , Jun Luo , Jianshu Li

Inspired by the thermal hysteresis of honey, we report an atypical temperature‑responsive strategy to overcome the strength-switchability trade-off in underwater adhesives. By programming the reversible polymerization-crystallization of the natural small-molecule thioctic acid (TA) using a long-chain alkylated TA derivative as “molecular pollen” and tris(2-carboxyethyl)phosphine (TCEP) as a stabilizer, we designed a robust yet highly reversible underwater adhesive. Upon mild heating, TA polymerizes into a metastable polyTA complex stabilized by TCEP and plasticized by the molecular pollen, maintaining a supercooled fluid state even below its crystallization temperature to enable thorough underwater wetting. Cooling underwater triggers depolymerization, releasing TA monomers that co‑crystallize with the molecular pollen to induce complete solidification with high cohesion. This mild thermal cycling enables wide-range cohesion modulation, yielding robust underwater adhesion (2.21 MPa on steel within 24 h) and high switching efficiency (>99.9 %) within a narrow temperature window (ΔT ≤ 30 °C). With honey-like thermal hysteresis near body temperature, the adhesive provides secure wound sealing and stable catheter fixation (≥7 d) in vivo, followed by minimal-trauma removal with reduced inflammation under gentle thermal stimulation. This sustainable biomimetic strategy resolves the “switchability conflict” in underwater adhesives, with promising applicability in medical device fixation, wearable electronics, and reversible assembly.

受蜂蜜热滞后的启发，我们报告了一种非典型的温度响应策略，以克服水下粘合剂中强度-可切换性的权衡。通过对天然小分子硫辛酸（TA）的可逆聚合结晶进行编程，以长链烷基化TA衍生物为“分子花粉”，以三（2-羧基乙基）膦（TCEP）为稳定剂，设计了一种坚固且高度可逆的水下粘合剂。在温和加热下，TA聚合成亚稳的多TA复合物，由TCEP稳定，并被分子花粉增塑化，即使低于其结晶温度也能保持过冷的流体状态，从而实现彻底的水下润湿。水下冷却触发解聚，释放TA单体，与分子花粉共结晶，诱导具有高凝聚力的完全凝固。这种温和的热循环可以实现大范围的内聚调节，在狭窄的温度窗口（ΔT≤30°C）内产生强大的水下粘附力（24小时内对钢产生2.21 MPa）和高开关效率（> 99.9%）。该粘合剂具有接近体温的蜂蜜样热滞性，在体内可提供安全的伤口密封和稳定的导管固定（≥7 d），随后在温和的热刺激下进行最小创伤去除并减少炎症。这种可持续的仿生策略解决了水下胶粘剂的“可切换性冲突”，在医疗器械固定、可穿戴电子产品和可逆组装方面具有广阔的应用前景。

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引用次数: 0

Ambient inkjet-printed PHOLEDs with record efficiency via dual-SAM engineering and eco-friendly solvent design 通过双sam工程和环保溶剂设计，环境喷墨打印的oled具有创纪录的效率

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.017

Sagnik Chowdhury , Keum-Jin Ko , Vinayak Vitthal Satale , Hyerin Kim , Sung-Ho Jin , Jae-Wook Kang

Inkjet printing offers a scalable and material-efficient route for fabricating organic light-emitting devices, yet solution-processed phosphorescent OLEDs (PHOLEDs) remain limited by interfacial instability, solvent incompatibility, and poor ambient processability. In this study, we report a high-performance, hole-transport layer (HTL)-free PHOLED fully fabricated under ambient conditions using an inkjet printing strategy based on eco-friendly solvents. A dual self-assembled monolayer (SAM) modification on the ITO anode, combining 2,3,4,5,6-pentafluorobenzoyl phosphonic acid and tricosafluorododecanoic acid, enables efficient charge injection without the need for conventional HTLs. Complementing this, a binary solvent system comprising environmentally benign components is engineered to suppress the coffee-ring effect and significantly improve film uniformity. Furthermore, a newly designed heteroleptic Ir(III) emitter with tailored solubilizing groups enhances ink compatibility and charge-transport properties. The resulting devices achieve a record-high external quantum efficiency of 16.8% under ambient processing conditions, marking a new benchmark for inkjet-printed PHOLEDs. This work demonstrates a synergistic approach to interfacial engineering and eco-conscious solvent design, offering a scalable, sustainable pathway toward high-efficiency, vacuum-free OLED technologies.

喷墨打印为制造有机发光器件提供了一种可扩展和材料效率高的途径，但溶液处理磷光oled （PHOLEDs）仍然受到界面不稳定性、溶剂不相容性和环境可加工性差的限制。在这项研究中，我们报告了一种高性能，无空穴传输层（html）的PHOLED，采用基于环保溶剂的喷墨打印策略，在环境条件下完全制造。在ITO阳极上进行双自组装单层（SAM）修饰，结合2,3,4,5,6-五氟苯甲酰膦酸和三氟十二烷酸，可以实现高效的电荷注入，而无需传统的HTLs。与此相辅相成的是，一种包含环保成分的二元溶剂系统被设计用来抑制咖啡环效应，并显著提高膜的均匀性。此外，新设计的具有定制增溶基团的异渗Ir（III）发射极提高了油墨兼容性和电荷输运性能。由此产生的器件在环境处理条件下实现了创纪录的16.8%的外部量子效率，标志着喷墨打印的oled的新基准。这项工作展示了界面工程和生态溶剂设计的协同方法，为高效、无真空的OLED技术提供了可扩展、可持续的途径。

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引用次数: 0

Break-down of the relationship between α-relaxation and equilibration in hydrostatically compressed metallic glasses 流体静力压缩金属玻璃中α-弛豫与平衡关系的破坏

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.011

Antoine Cornet , Jie Shen , Alberto Ronca , Shubin Li , Nico Neuber , Maximilian Frey , Eloi Pineda , Thierry Deschamps , Christine Martinet , Sylvie Le Floch , Daniele Cangialosi , Yuriy Chushkin , Federico Zontone , Marco Cammarata , Gavin B.M. Vaughan , Marco di Michiel , Gaston Garbarino , Ralf Busch , Isabella Gallino , Celine Goujon , Beatrice Ruta

Glasses encode the memory of any thermo-mechanical treatment applied to them. This ability is associated to the existence of a myriad of metastable amorphous states which can be probed through different experimental pathways. It is usually assumed that this memory can be erased in the supercooled liquid, and that this process occurs on a time scale controlled by the α-relaxation. We find that this assumption does not apply for hydrostatically compressed glasses. Annealing under pressure a prototypical metallic glass can irreversibly modify its dynamics, thermodynamics and structure, reduce the atomic mobility and lead to structural modifications of the first coordination shells which reduce the thermal stability with respect to a glass annealed in absence of pressure. When heated above their glass transition temperature, these compressed glasses do not convert into the pristine supercooled liquid, implying the existence of an additional process, beyond the α-relaxation, contributing to the equilibrium recovery of the material. These results establish pressure as a powerful tool for engineering non-equilibrium glassy materials with tailored properties, while deepening our understanding of relaxation dynamics in disordered systems under extreme conditions.

眼镜能将任何热处理的记忆编码。这种能力与无数亚稳态非晶态的存在有关，这些亚稳态非晶态可以通过不同的实验途径进行探测。通常认为这种记忆可以在过冷的液体中被擦除，并且这一过程在α-弛豫控制的时间尺度上发生。我们发现这个假设不适用于流体静力压缩玻璃。压力退火可以不可逆地改变原型金属玻璃的动力学、热力学和结构，降低原子迁移率并导致第一配位壳的结构改变，从而降低相对于无压力退火的玻璃的热稳定性。当加热到高于玻璃化转变温度时，这些压缩玻璃不会转化为原始的过冷液体，这意味着除了α-弛豫之外，还存在一个额外的过程，有助于材料的平衡恢复。这些结果确立了压力作为具有定制特性的非平衡玻璃材料工程的有力工具，同时加深了我们对极端条件下无序系统松弛动力学的理解。

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引用次数: 0

Material reformation and opportunities created by tetraamino-p-benzoquinone 四氨基对苯醌的物质改造与机遇

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.010

Qun Liu , Haoyu Guo , Chengliang Wang

Conjugated organic/polymeric materials with multi-functional groups are superior in material reformation and diverse applications. However, the combination of conjugation and the functional groups bring inherent complexities, leading to different reaction modes from non-conjugated systems, uncontrolled reactions, doubtful performance and ambiguous structure–property relationships. As a typical example, tetraamino-p-benzoquinone (TABQ) is a recent star material due to its conjugated core and rich functional groups, which has been not only applied in various applications but also used to construct abundant novel materials including small molecules, oligomers, polymers, covalent-organic frameworks and metal–organic frameworks through synthesis control and topological construction. By delving into the possibilities from TABQ, this review aims to draw attention to the cautious molecular design of conjugated materials, avoid the misunderstandings originating from the unexpected reactions of the multi-functional groups, evoke patience on the insightful structure–property relationship, and inspire new opportunities for the creation of more functionalized material systems.

具有多官能团的共轭有机高分子材料在材料改造和应用方面具有优势。然而，共轭与官能团的结合带来了固有的复杂性，导致了与非共轭体系不同的反应方式、不受控制的反应、可疑的性能和不明确的结构-性质关系。以四氨基对苯醌（TABQ）为例，由于其共轭核和丰富的官能团，TABQ是近年来发展起来的新星材料，不仅得到了广泛的应用，而且通过合成控制和拓扑构建，可以构建小分子、低聚物、聚合物、共价有机框架和金属有机框架等丰富的新型材料。通过深入探讨TABQ的可能性，本文旨在引起人们对共轭材料的谨慎分子设计的关注，避免因多官能团的意外反应而引起的误解，唤起人们对深刻的结构-性质关系的耐心，并为创造更功能化的材料体系提供新的机会。

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引用次数: 0

Advancing analysis of differential scanning calorimetry data – Converging DSC and AI 差示扫描量热数据的先进分析——DSC和AI的融合

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.036

B.L. Dargaville , T. Ayyachi , D.W. Hutmacher

Differential scanning calorimetry (DSC) is a prominent analytical technique in materials science, offering detailed insights into the thermal properties and behavior of materials. DSC provides valuable information for understanding material composition, structure, and performance by measuring the heat flow associated with thermal events. Interpreting DSC curves is a complex process that requires substantial expertise, and misinterpretation can lead to inaccurate conclusions about material properties. Integrating artificial intelligence (AI) into DSC presents a transformative opportunity to significantly enhance the accuracy, precision, and reliability of thermal analysis. By employing advanced AI algorithms, researchers can analyze DSC data in real time, allowing immediate insights into thermal transitions, such as glass transition, crystallization, and melting. This review outlines how the convergence of DSC and AI can not only expedite the research process but also standardize data interpretation, minimize human error, and reduce reliance on specialized operator expertise, thereby empowering non-experts to interpret DSC data with greater confidence and accuracy. This integration enhances the accessibility, reproducibility, and credibility of thermal data derived from advanced thermal analysis techniques across various scientific and industrial sectors.

差示扫描量热法（DSC）是材料科学中一项重要的分析技术，提供了对材料热性能和行为的详细见解。DSC通过测量与热事件相关的热流，为理解材料的组成、结构和性能提供了有价值的信息。解释DSC曲线是一个复杂的过程，需要大量的专业知识，误解可能导致对材料特性的不准确结论。将人工智能（AI）集成到DSC中提供了一个变革性的机会，可以显着提高热分析的准确性，精度和可靠性。通过采用先进的人工智能算法，研究人员可以实时分析DSC数据，从而可以立即了解热转变，如玻璃化转变、结晶和熔化。本文概述了DSC和人工智能的融合不仅可以加快研究过程，还可以标准化数据解释，最大限度地减少人为错误，减少对专业操作员专业知识的依赖，从而使非专家能够更有信心和更准确地解释DSC数据。这种集成增强了来自各种科学和工业部门的先进热分析技术的热数据的可访问性、可重复性和可信度。

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引用次数: 0

Synergizing ROS-biocatalysis and biofilm penetration via photothermal artificial enzymes with atomic homojunction sites to eradicate drug-resistant bacterial infections 利用具有原子同质结位点的光热人工酶协同ros -生物催化和生物膜渗透以根除耐药细菌感染

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.003

Xizheng Wu , Zhenyu Xing , Jiangge Li , Zhiying Ding , Lingnuo Fan , Mao Wang , Tian Ma , Chong Cheng , Weifeng Zhao , Changsheng Zhao

The treatment of biofilm-associated drug-resistant bacterial infections remains a formidable clinical challenge, primarily due to the limited permeability of therapeutic agents through the dense extracellular matrix and the inherent drug resistance of biofilm-embedded microorganisms. Here, to overcome this challenge, we report the design of an atomic Fe-O-Mo/Fe-S-Mo homojunction photothermal nanosheet (Fe-HJPS) to synergize reactive oxygen species (ROS)-biocatalysis and biofilm penetration for eradicating drug-resistant bacterial infections. Spectroscopic and computational analyses reveal that the homojunction sites in the Fe-HJPS, comprising asymmetric Fe-S-Mo/Fe-O-Mo coordinations around Fe centers, downshift the high d-p hybrid orbital energy level compared to the original symmetric Fe-S-Mo coordination. This optimization enhances the adsorption affinity of oxygen intermediates and improves ROS-biocatalytic activities. Notably, under near-infrared (NIR) irradiation, the Fe-HJPS generates localized heat and disturbs the extracellular polymeric substances (EPS) in biofilms to increase the permeability of bacterial membranes, thereby facilitating ROS influx into bacterial cells. This dual-action mechanism of ROS production and biofilm penetration enables effective biofilm eradication at ultralow concentration (40 μg·mL⁻¹), demonstrating superior efficacy against drug-resistant infections in both in vitro and in vivo models. Our findings establish atomic-scale homojunction in photothermal artificial enzymes as a versatile strategy for designing non-antibiotic antimicrobial nanomaterials that overcome drug-resistant bacterial infections.

生物膜相关耐药细菌感染的治疗仍然是一项艰巨的临床挑战，主要是由于治疗剂通过致密的细胞外基质的渗透性有限以及生物膜内微生物固有的耐药性。为了克服这一挑战，我们设计了一种原子Fe-O-Mo/Fe-S-Mo同质结光热纳米片（Fe-HJPS），以协同活性氧（ROS）生物催化和生物膜渗透，消除耐药细菌感染。光谱分析和计算分析表明，Fe- hjps中由Fe中心周围的不对称Fe- s - mo /Fe- o - mo配位组成的同结位与原来对称的Fe- s - mo配位相比，降低了高d-p杂化轨道的能级。该优化提高了氧中间体的吸附亲和力，提高了活性氧生物催化活性。值得注意的是，在近红外（NIR）照射下，Fe-HJPS产生局部热，扰乱生物膜中的胞外聚合物（EPS），增加细菌膜的通透性，从而促进ROS流入细菌细胞。这种ROS生成和穿透生物膜的双重作用机制能够在超低浓度（40 μg·mL−1）下有效清除生物膜，在体外和体内模型中均显示出对耐药感染的卓越疗效。我们的研究结果建立了光热人工酶的原子尺度同质结，作为设计克服耐药细菌感染的非抗生素抗菌纳米材料的通用策略。

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引用次数: 0

Locking aggregation states in tough hydrogels through protective domain formation 通过形成保护结构域锁定坚韧水凝胶中的聚集态

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2025.12.005

Hao Nan Qiu , Chuan Wei Zhang , Lixin Dai , Yichen Yan , Ping He , Ruoyi Ke , Xiaobing Zuo , Hua Zhou , Ximin He

Tough hydrogels based on physical crosslinking have attracted tremendous attention due to their excellent mechanical properties achieved through controlled polymer chain aggregation via various processing methods. However, the reversible nature of these physical interactions leads to severe mechanical degradation in aqueous environments, where water molecules competitively disrupt hydrogen bonds and dissolve aggregated structures, fundamentally limiting their practical applications. Herein, we propose a strategy to construct protective domains around physical crosslinks that effectively stabilize the network while preserving energy dissipation capabilities. Using poly(vinyl alcohol) (PVA) as a model system, we implement this design through sequential dehydration-induced crystallization and homogeneous free-radical crosslinking (FRC). The resulting protective domains—chemically-crosslinked loose aggregates surrounding crystallites—serve dual functions: shielding physical crosslinks from solvent-induced disruption and storing hidden chain length that enhances extensibility during deformation. Compared to unprotected physically crosslinked hydrogels, this strategy achieves 2.4-fold enhancement in elastic modulus, 2.1-fold increase in breaking strain, and 4.8-fold improvement in toughness, while dramatically improving environmental stability--the mechanical strength retention increases from ∼ 20 % to > 80 % after aqueous immersion, with volume expansion reduced from typical 20–30 % to less than 5 %. Microstructural characterization confirms the coexistence of protected crystallites and loose aggregates. The hydrogel is successfully employed as an electrolyte to construct zinc-ion batteries that feature superior cycling performance, enabled by the exceptional environmental stability and strong structural endurance of the hydrogel. This strategy proves generalizable to various physically crosslinked systems, offering a universal design principle for creating mechanically robust and environmentally stable hydrogels.

基于物理交联的韧性水凝胶由于其优异的力学性能而受到广泛关注，这些性能是通过各种加工方法控制聚合物链聚集而获得的。然而，这些物理相互作用的可逆性导致水环境中严重的机械降解，水分子竞争性地破坏氢键并溶解聚集结构，从根本上限制了它们的实际应用。在此，我们提出了一种策略，在物理交联周围构建保护域，有效地稳定网络，同时保持能量耗散能力。我们以聚乙烯醇（PVA）为模型体系，通过连续脱水诱导结晶和均相自由基交联（FRC）来实现这一设计。由此产生的保护结构域——围绕晶体的化学交联松散聚集体——具有双重功能：保护物理交联免受溶剂引起的破坏，并存储隐藏的链长度，从而增强变形过程中的可扩展性。与无保护的物理交联水凝胶相比，该策略的弹性模量提高了2.4倍，断裂应变提高了2.1倍，韧性提高了4.8倍，同时显著提高了环境稳定性——水浸后机械强度保有率从20%增加到80%，体积膨胀从典型的20 - 30%降低到5%以下。微观结构表征证实了保护结晶和松散聚集体的共存。由于水凝胶优异的环境稳定性和强大的结构耐久性，水凝胶成功地用作锌离子电池的电解质，具有卓越的循环性能。事实证明，该策略适用于各种物理交联体系，为制造机械坚固且环境稳定的水凝胶提供了通用设计原则。

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引用次数: 0

Strategic defect engineering in ceria interlayer for high-performing solid oxide electrochemical cells 高性能固体氧化物电化学电池中二氧化铈中间层的战略性缺陷工程

IF 22 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2026-01-01 DOI: 10.1016/j.mattod.2026.01.002

Hyeongmin Yu , Incheol Jeong , Sang Won Lee , Hansu Chang , Seeun Oh , Tae Ho Shin , Kang Taek Lee

Solid oxide electrochemical cells (SOCs) represent a transformative platform for the efficient and sustainable interconversion between chemical and electrical energy, enabling green hydrogen production and high-efficiency power generation. However, their widespread deployment is constrained by high operating temperatures, as performance degrades sharply at reduced temperatures especially due to increased polarization and ohmic resistances at the oxygen electrode/electrolyte interface. Herein, we present a rationally engineered, defect-rich thin-film ceria interlayer designed to enhance interfacial oxygen exchange kinetics and shorten ion transport pathways, effectively mitigating both polarization and bulk ohmic losses. Density functional theory calculations reveal that excess Gd doping weakens the cation-oxygen bonding and introduces tensile lattice strain, which synergistically lower the oxygen vacancy formation energy and promote vacancy clustering at the surface. These effects enhance both oxygen storage/release capacity and the kinetics of oxygen incorporation and evolution. When incorporated into SOCs, the developed defect-rich ceria interlayer enables exceptional electrochemical performance, achieving a peak power density of 3.00 W/cm² in fuel cell mode and a current density of 1.85 A/cm² in electrolysis mode at 700°C, significantly outperforming conventional ceria-based interlayers. This work provides new design principles for interlayer engineering in SOCs, and offers a promising pathway toward next-generation energy conversion technologies.

固体氧化物电化学电池（soc）代表了化学和电能之间高效和可持续相互转换的变革性平台，实现了绿色制氢和高效发电。然而，由于氧电极/电解质界面的极化和欧姆电阻增加，其性能在低温下急剧下降，因此它们的广泛部署受到高温的限制。在此，我们提出了一种合理设计的，富含缺陷的薄膜铈中间层，旨在增强界面氧交换动力学和缩短离子传输途径，有效地减轻极化和体欧姆损失。密度泛函理论计算表明，过量的Gd掺杂削弱了阳离子-氧键并引入了拉伸晶格应变，从而协同降低了氧空位形成能，促进了空位在表面聚集。这些作用增强了氧的储存/释放能力以及氧的结合和演化动力学。当集成到soc中时，所开发的富含缺陷的二氧化铈中间层具有卓越的电化学性能，在燃料电池模式下可实现3.00 W/cm2的峰值功率密度，在700°C电解模式下可实现1.85 a /cm2的电流密度，显著优于传统的二氧化铈中间层。这项工作为soc的层间工程提供了新的设计原则，并为下一代能量转换技术提供了一条有希望的途径。

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