首页 > 最新文献

Materials Horizons最新文献

英文 中文
Hybrid metamaterials for decoupled electromagnetic-acoustic wave manipulation: achieving four negative constitutive parameters. 去耦电磁声波操纵的杂化超材料:实现四个负本构参数。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-18 DOI: 10.1039/d5mh01858g
Zhaolun Yu, Tian Gan, Xiaole Wang, Chunyu Zhao, Zhenyu Huang, Xudong Luo

In the context of metamaterials, decoupled access to the four constitutive parameters (permittivity, permeability, mass density, and bulk modulus) using a single architecture can unlock substantial design freedom, thereby enabling possibilities for a wide range of electromagnetic and acoustic wave manipulation applications. Herein, we propose a modular replaceable design paradigm for hybrid metamaterials to independently control electromagnetic and acoustic properties within a unified metamaterial unit cell. By arranging printed circuit board traces into an interleaved, meandering lattice, the proposed hybrid metamaterial can simultaneously generate microwave resonances for tuning of negative permittivity and permeability while acting as rigid acoustic boundaries of space-coiled air channels to produce negative mass density and bulk modulus. This hybrid metamaterial is further experimentally demonstrated to realise the simultaneous negative refraction of electromagnetic and acoustic waves. Our design paradigm represents a promising pathway toward advanced hybrid metamaterials, potentially enabling unprecedented functionalities in wave manipulation, sensing, and integrated electromagnetic-acoustic devices.

在超材料的背景下,使用单一架构解耦访问四个本构参数(介电常数、磁导率、质量密度和体积模量)可以解锁大量的设计自由度,从而为广泛的电磁波和声波操纵应用提供了可能性。在此,我们提出了一种模块化的可替换设计范式,用于混合超材料在统一的超材料单元胞内独立控制电磁和声学特性。通过将印刷电路板迹线排列成交错的蜿蜒晶格,所提出的混合超材料可以同时产生微波共振以调谐负介电常数和磁导率,同时作为空间卷曲空气通道的刚性声学边界以产生负质量密度和体积模量。实验进一步证明了这种混合超材料可以同时实现电磁波和声波的负折射。我们的设计范例代表了一条通往先进混合超材料的有希望的途径,可能在波操纵、传感和集成电磁声设备方面实现前所未有的功能。
{"title":"Hybrid metamaterials for decoupled electromagnetic-acoustic wave manipulation: achieving four negative constitutive parameters.","authors":"Zhaolun Yu, Tian Gan, Xiaole Wang, Chunyu Zhao, Zhenyu Huang, Xudong Luo","doi":"10.1039/d5mh01858g","DOIUrl":"https://doi.org/10.1039/d5mh01858g","url":null,"abstract":"<p><p>In the context of metamaterials, decoupled access to the four constitutive parameters (permittivity, permeability, mass density, and bulk modulus) using a single architecture can unlock substantial design freedom, thereby enabling possibilities for a wide range of electromagnetic and acoustic wave manipulation applications. Herein, we propose a modular replaceable design paradigm for hybrid metamaterials to independently control electromagnetic and acoustic properties within a unified metamaterial unit cell. By arranging printed circuit board traces into an interleaved, meandering lattice, the proposed hybrid metamaterial can simultaneously generate microwave resonances for tuning of negative permittivity and permeability while acting as rigid acoustic boundaries of space-coiled air channels to produce negative mass density and bulk modulus. This hybrid metamaterial is further experimentally demonstrated to realise the simultaneous negative refraction of electromagnetic and acoustic waves. Our design paradigm represents a promising pathway toward advanced hybrid metamaterials, potentially enabling unprecedented functionalities in wave manipulation, sensing, and integrated electromagnetic-acoustic devices.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145772882","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Scalable and sustainable manufacturing of intermetallic nanocrystals for economical water splitting. 用于经济水分解的可扩展和可持续的金属间纳米晶体制造。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01854d
Mingjin Cui, Haijiao Liu, Ke Chen, Xinwei Shi, Bo Xu, Chenlu Jiang, Dehui Li, Ding Yuan, Yuhai Dou, Chao Wu, Menghao Yang, Shixue Dou, Yu Ding

Intermetallic nanocatalysts are pivotal for advancing energy conversion and storage technologies. However, their industrial-scale synthesis is fundamentally hindered by the difficulty of maintaining precise compositional and structural control. Here, we introduce a universal phase-engineering strategy, actualized through a continuous roll-flow radiative heating platform that enables the one-step, scalable, and controllable synthesis of highly ordered intermetallic nanocatalysts. This innovative technique demonstrates remarkable versatility, rendering precise fabrication of intermetallic nanocrystals across a vast compositional landscape. Crucially, by modulating key kinetic parameters during synthesis, we achieve precise control over ordering arrangement with fine-tuning of catalytic performance. As a proof of concept, we demonstrate the scalable and sustainable synthesis of nickel-iron intermetallic (Ni3Fe) nanocatalysts with a predominant L12-ordered crystal structure for efficient alkaline water splitting. The resulting catalyst exhibits exceptional electrocatalytic activity, reaching a current density of 10 mA cm-2 at a low overpotential of 200.2 mV, a performance that rivals the commercial iridium dioxide (IrO2) benchmark (199.2 mV). Moreover, it shows outstanding long-term durability, with 99.9% current retention over 140 hours and negligible metal leaching. A comprehensive techno-economic evaluation reveals that the hydrogen production cost is strongly dependent on current density, projecting a highly competitive H2 price as low as $2.33 kg-1 at 1.0 A cm-2. This work is expected to provide advanced technology for scalable, sustainable, and continuous manufacturing of intermetallic nanocrystals for economical water splitting.

金属间纳米催化剂是推进能量转换和存储技术的关键。然而,由于难以保持精确的成分和结构控制,它们的工业规模合成从根本上受到阻碍。在这里,我们介绍了一种通用的相工程策略,通过连续滚流辐射加热平台实现了一步,可扩展和可控的高度有序的金属间纳米催化剂合成。这种创新的技术展示了非凡的多功能性,可以在广阔的组成景观中精确地制造金属间纳米晶体。至关重要的是,通过调节合成过程中的关键动力学参数,我们可以通过微调催化性能来精确控制有序排列。作为概念证明,我们展示了可扩展和可持续合成的镍铁金属间化合物(Ni3Fe)纳米催化剂,其主要晶体结构为l12有序,用于高效的碱性水分解。所得到的催化剂表现出优异的电催化活性,在200.2 mV的低过电位下达到10 mA cm-2的电流密度,其性能可与商业二氧化铱(IrO2)基准(199.2 mV)相媲美。此外,它具有出色的长期耐久性,在140小时内保持99.9%的电流,金属浸出可以忽略不计。一项综合技术经济评估显示,氢气生产成本在很大程度上取决于电流密度,预计在1.0 A cm-2下,氢气价格将低至2.33美元/ kg-1,具有很强的竞争力。这项工作有望为可扩展、可持续和连续制造用于经济水分解的金属间纳米晶体提供先进技术。
{"title":"Scalable and sustainable manufacturing of intermetallic nanocrystals for economical water splitting.","authors":"Mingjin Cui, Haijiao Liu, Ke Chen, Xinwei Shi, Bo Xu, Chenlu Jiang, Dehui Li, Ding Yuan, Yuhai Dou, Chao Wu, Menghao Yang, Shixue Dou, Yu Ding","doi":"10.1039/d5mh01854d","DOIUrl":"https://doi.org/10.1039/d5mh01854d","url":null,"abstract":"<p><p>Intermetallic nanocatalysts are pivotal for advancing energy conversion and storage technologies. However, their industrial-scale synthesis is fundamentally hindered by the difficulty of maintaining precise compositional and structural control. Here, we introduce a universal phase-engineering strategy, actualized through a continuous roll-flow radiative heating platform that enables the one-step, scalable, and controllable synthesis of highly ordered intermetallic nanocatalysts. This innovative technique demonstrates remarkable versatility, rendering precise fabrication of intermetallic nanocrystals across a vast compositional landscape. Crucially, by modulating key kinetic parameters during synthesis, we achieve precise control over ordering arrangement with fine-tuning of catalytic performance. As a proof of concept, we demonstrate the scalable and sustainable synthesis of nickel-iron intermetallic (Ni<sub>3</sub>Fe) nanocatalysts with a predominant L1<sub>2</sub>-ordered crystal structure for efficient alkaline water splitting. The resulting catalyst exhibits exceptional electrocatalytic activity, reaching a current density of 10 mA cm<sup>-2</sup> at a low overpotential of 200.2 mV, a performance that rivals the commercial iridium dioxide (IrO<sub>2</sub>) benchmark (199.2 mV). Moreover, it shows outstanding long-term durability, with 99.9% current retention over 140 hours and negligible metal leaching. A comprehensive techno-economic evaluation reveals that the hydrogen production cost is strongly dependent on current density, projecting a highly competitive H<sub>2</sub> price as low as $2.33 kg<sup>-1</sup> at 1.0 A cm<sup>-2</sup>. This work is expected to provide advanced technology for scalable, sustainable, and continuous manufacturing of intermetallic nanocrystals for economical water splitting.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766660","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Construction of hierarchical 2D/2D few-layered MoS2/S-doped g-C3N4 heterojunctions for enhanced photocatalytic formaldehyde removal. 多层2D/2D少层MoS2/ s掺杂g-C3N4异质结的构建增强光催化甲醛去除。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01490e
Yihao Duan, Haihua Wang, Guiqiang Fei, Yu Wang, Liyu Sun

Modification of graphitic carbon nitride (g-C3N4) with semiconductor nanomaterials has been widely investigated as an effective method to enhance its photocatalytic activity. However, the construction of efficient g-C3N4-based heterojunction photocatalysts via an environmentally benign method remains critical. Herein, a two-dimensional (2D) few-layered MoS2/S-doped g-C3N4 hierarchical heterojunction was successfully synthesized by a simple strategy via combining small molecule-assisted liquid exfoliation, calcination and hydrothermal strategy, which was subsequently utilized for photocatalytic formaldehyde removal. The evaluation of the photocatalytic degradation reaction showed that the as-prepared 2D/2D MoS2/S-doped g-C3N4 photocatalysts exhibited superior photocatalytic activity compared to pristine g-C3N4 and S-doped g-C3N4 alone, which was attributed to the intimate interface and rapid charge transfer pathways. This heterojunction structure suppresses the excited electron-hole pair recombination within g-C3N4, which optimally enhances the photodegradation activity owing to high electron-hole pair separation efficiency. The few-layer MoS2 nanosheets play an irreplaceable role due to their unique molybdenum-sulfur atomic arrangement, thereby displaying the superior electronic properties of few-layer or even monolayer nanosheets, which make them an important transfer medium for photoexcited electrons. Meanwhile, S doping effectively modulates the band gap of g-C3N4 and introduces sufficient structural defects to inhibit electron-hole recombination. Moreover, the synthesis employs efficient and non-hazardous reagents, and the resulting catalysts exhibit outstanding stability and recyclability for pollutant degradation.

利用半导体纳米材料对石墨氮化碳(g-C3N4)进行改性是提高其光催化活性的一种有效方法,已被广泛研究。然而,通过环境友好的方法构建高效的g- c3n4基异质结光催化剂仍然是关键。本文采用小分子辅助液体剥离、煅烧和水热相结合的简单策略,成功合成了二维(2D)少层MoS2/ s掺杂g-C3N4层次化异质结,并将其用于光催化甲醛去除。光催化降解反应的评价表明,制备的2D/2D MoS2/ s掺杂g-C3N4光催化剂与原始g-C3N4和单独s掺杂g-C3N4相比,表现出更强的光催化活性,这归因于其紧密的界面和快速的电荷转移途径。这种异质结结构抑制了g-C3N4内部受激发的电子-空穴对复合,从而提高了g-C3N4的光降解活性。少层MoS2纳米片以其独特的钼硫原子排列方式发挥着不可替代的作用,从而显示出少层甚至单层纳米片优越的电子性能,成为光激发电子的重要传递介质。同时,S掺杂有效地调节了g-C3N4的带隙,引入了足够的结构缺陷,抑制了电子-空穴复合。此外,该合成方法采用了高效、无害的试剂,所得到的催化剂具有优异的稳定性和可回收性,可降解污染物。
{"title":"Construction of hierarchical 2D/2D few-layered MoS<sub>2</sub>/S-doped g-C<sub>3</sub>N<sub>4</sub> heterojunctions for enhanced photocatalytic formaldehyde removal.","authors":"Yihao Duan, Haihua Wang, Guiqiang Fei, Yu Wang, Liyu Sun","doi":"10.1039/d5mh01490e","DOIUrl":"https://doi.org/10.1039/d5mh01490e","url":null,"abstract":"<p><p>Modification of graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) with semiconductor nanomaterials has been widely investigated as an effective method to enhance its photocatalytic activity. However, the construction of efficient g-C<sub>3</sub>N<sub>4</sub>-based heterojunction photocatalysts <i>via</i> an environmentally benign method remains critical. Herein, a two-dimensional (2D) few-layered MoS<sub>2</sub>/S-doped g-C<sub>3</sub>N<sub>4</sub> hierarchical heterojunction was successfully synthesized by a simple strategy <i>via</i> combining small molecule-assisted liquid exfoliation, calcination and hydrothermal strategy, which was subsequently utilized for photocatalytic formaldehyde removal. The evaluation of the photocatalytic degradation reaction showed that the as-prepared 2D/2D MoS<sub>2</sub>/S-doped g-C<sub>3</sub>N<sub>4</sub> photocatalysts exhibited superior photocatalytic activity compared to pristine g-C<sub>3</sub>N<sub>4</sub> and S-doped g-C<sub>3</sub>N<sub>4</sub> alone, which was attributed to the intimate interface and rapid charge transfer pathways. This heterojunction structure suppresses the excited electron-hole pair recombination within g-C<sub>3</sub>N<sub>4</sub>, which optimally enhances the photodegradation activity owing to high electron-hole pair separation efficiency. The few-layer MoS<sub>2</sub> nanosheets play an irreplaceable role due to their unique molybdenum-sulfur atomic arrangement, thereby displaying the superior electronic properties of few-layer or even monolayer nanosheets, which make them an important transfer medium for photoexcited electrons. Meanwhile, S doping effectively modulates the band gap of g-C<sub>3</sub>N<sub>4</sub> and introduces sufficient structural defects to inhibit electron-hole recombination. Moreover, the synthesis employs efficient and non-hazardous reagents, and the resulting catalysts exhibit outstanding stability and recyclability for pollutant degradation.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766710","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Suppression of interfacial layers in ZrO2/TiN capacitors by atomic layer deposition using ligand-engineered Zr precursors for scalable DRAM. 用配体工程Zr前驱体原子层沉积抑制可扩展DRAM中ZrO2/TiN电容器界面层。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01502b
Hyeongjun Kim, Juan Hong, Sangyeon Jeong, Kyunghun Lyu, Seungmin Jo, Seokho Cho, Juhyeong Kim, Byung-Kwan Kim, Jin-Sik Kim, Woongkyu Lee

As dynamic random-access memory continues to scale down, the feasible physical thickness of the capacitor dielectric layer continuously decreases, thus, controlling the low-k interfacial layer formed at the ZrO2 dielectric/TiN electrode interface is becoming crucial. The interfacial layer reduces the capacitance density and increases the leakage current density, and both of them contribute to the degradation of the overall properties of the capacitor. In this study, two precursors were compared: the commonly used Cp-based Zr precursor, Cp-Zr(NMe2)3 [Cp-Zr] and the novel MePrCp-Zr(NMe2)3 [MePrCp-Zr] precursor, with the two terminal hydrogens of the Cp ligand substituted with Me and Pr groups. MePrCp-Zr was confirmed to suppress the formation of low-k interfacial layers such as TiOx or TiOxNy at the initial ZrO2 growth stage, owing to its higher reactivity than Cp-Zr. Furthermore, analysis of oxidation behavior using TiN and Ru bottom electrodes clearly revealed that the application of MePrCp-Zr led to improved interfacial sharpness compared to Cp-Zr. Electrical properties also confirmed enhanced interfacial properties, indicating that the equivalent oxide thickness decreased by 0.38 nm with the MePrCp-Zr precursor compared to Cp-Zr. This ligand-engineering strategy provides a scalable approach to achieving ultrathin high-k dielectrics with stable interfaces, enabling reliable capacitor integration for next-generation DRAM and advanced logic technologies.

随着动态随机存取存储器的不断缩小,电容器介电层的可行物理厚度不断减小,因此控制在ZrO2介电/TiN电极界面处形成的低k界面层变得至关重要。界面层降低了电容密度,增加了漏电流密度,两者都导致了电容器整体性能的下降。本研究比较了两种前体:常用的Cp基Zr前体Cp-Zr(NMe2)3 [Cp-Zr]和新型的MePrCp-Zr(NMe2)3 [MePrCp-Zr], Cp配体的两个末端氢被Me和Pr取代。由于MePrCp-Zr比Cp-Zr具有更高的反应活性,因此在ZrO2生长初期,MePrCp-Zr抑制了TiOx或TiOxNy等低k界面层的形成。此外,对TiN和Ru底电极的氧化行为分析清楚地表明,与Cp-Zr相比,MePrCp-Zr的应用提高了界面锐度。电学性能也证实了界面性能的增强,表明与Cp-Zr相比,MePrCp-Zr前驱体的等效氧化物厚度减少了0.38 nm。这种配体工程策略提供了一种可扩展的方法来实现具有稳定接口的超薄高k介电体,为下一代DRAM和先进的逻辑技术提供可靠的电容器集成。
{"title":"Suppression of interfacial layers in ZrO<sub>2</sub>/TiN capacitors by atomic layer deposition using ligand-engineered Zr precursors for scalable DRAM.","authors":"Hyeongjun Kim, Juan Hong, Sangyeon Jeong, Kyunghun Lyu, Seungmin Jo, Seokho Cho, Juhyeong Kim, Byung-Kwan Kim, Jin-Sik Kim, Woongkyu Lee","doi":"10.1039/d5mh01502b","DOIUrl":"https://doi.org/10.1039/d5mh01502b","url":null,"abstract":"<p><p>As dynamic random-access memory continues to scale down, the feasible physical thickness of the capacitor dielectric layer continuously decreases, thus, controlling the low-<i>k</i> interfacial layer formed at the ZrO<sub>2</sub> dielectric/TiN electrode interface is becoming crucial. The interfacial layer reduces the capacitance density and increases the leakage current density, and both of them contribute to the degradation of the overall properties of the capacitor. In this study, two precursors were compared: the commonly used Cp-based Zr precursor, Cp-Zr(NMe<sub>2</sub>)<sub>3</sub> [Cp-Zr] and the novel MePrCp-Zr(NMe<sub>2</sub>)<sub>3</sub> [MePrCp-Zr] precursor, with the two terminal hydrogens of the Cp ligand substituted with Me and Pr groups. MePrCp-Zr was confirmed to suppress the formation of low-<i>k</i> interfacial layers such as TiO<sub><i>x</i></sub> or TiO<sub><i>x</i></sub>N<sub><i>y</i></sub> at the initial ZrO<sub>2</sub> growth stage, owing to its higher reactivity than Cp-Zr. Furthermore, analysis of oxidation behavior using TiN and Ru bottom electrodes clearly revealed that the application of MePrCp-Zr led to improved interfacial sharpness compared to Cp-Zr. Electrical properties also confirmed enhanced interfacial properties, indicating that the equivalent oxide thickness decreased by 0.38 nm with the MePrCp-Zr precursor compared to Cp-Zr. This ligand-engineering strategy provides a scalable approach to achieving ultrathin high-<i>k</i> dielectrics with stable interfaces, enabling reliable capacitor integration for next-generation DRAM and advanced logic technologies.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Dendrimers with a far-red NDI fluorescent core for efficient and traceable gene and RNA delivery. 具有远红色NDI荧光核心的树状大分子,用于高效和可追溯的基因和RNA传递。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01468a
Hariharan Moorthy, Madhu Ramesh, Elumalai Premalatha, Thimmaiah Govindaraju

Dendrimer-based nucleic acid (NA) delivery systems have attracted significant attention due to their synthetic versatility, monodispersity, nuclease resistance, high payload release, and transfection efficiency. The conventional dendrimers are non-fluorescent, limiting their utility in real-time tracking and monitoring of drug delivery. Although terminal functionalization with fluorophores can partially address this issue, it often alters critical physicochemical properties and transfection efficiency. In this study, we report the design and development of far-red fluorescent dendrimers with a naphthalene diimide (NDI)-core for efficient and traceable gene and RNA delivery. These intrinsically fluorescent dendrimers enable real-time monitoring of cellular uptake and delivery. The NDI G3 formulation effectively condenses DNA, protects it from DNase-mediated degradation, and facilitates efficient transfection in cells. Therapeutically, NDI G3 demonstrated efficient glutathione peroxidase 4 (GPX4) siRNA delivery, comparable to PAMAM G3 and Lipofectamine 3000. Notably, the NDI G3-Ca2+-GPX4 siRNA-FINO2 formulation sensitizes human colon cancer-derived cells to ferroptosis, synergistically annihilating cancer cells compared to treatment with FINO2 alone. The intrinsically far-red fluorescent NDI G3 dendrimer with a dynamic fluorescence response developed for the combinatorial delivery of siRNA and drug molecules offers a generalized framework for designing next-generation far-red fluorescent dendrimers for nucleic acid therapeutics and theranostic applications.

树突状核酸(NA)递送系统因其合成多功能性、单分散性、核酸酶抗性、高负载释放和转染效率而受到广泛关注。传统的树状大分子是非荧光的,限制了它们在实时跟踪和监测药物输送方面的应用。虽然用荧光团的末端功能化可以部分解决这个问题,但它经常改变关键的物理化学性质和转染效率。在这项研究中,我们报道了设计和开发具有萘二亚胺(NDI)核的远红色荧光树状大分子,用于高效和可追溯的基因和RNA传递。这些本质上荧光的树状大分子能够实时监测细胞摄取和递送。NDI G3配方有效地浓缩DNA,保护DNA免受DNA酶介导的降解,并促进细胞内高效转染。在治疗方面,NDI G3表现出高效的谷胱甘肽过氧化物酶4 (GPX4) siRNA递送,与PAMAM G3和Lipofectamine 3000相当。值得注意的是,与单独使用FINO2治疗相比,NDI G3-Ca2+-GPX4 siRNA-FINO2制剂使人结肠癌来源的细胞对铁凋亡敏感,协同湮灭癌细胞。具有动态荧光响应的内在远红荧光NDI G3树状大分子用于siRNA和药物分子的组合递送,为设计用于核酸治疗和治疗应用的下一代远红荧光树状大分子提供了一个通用框架。
{"title":"Dendrimers with a far-red NDI fluorescent core for efficient and traceable gene and RNA delivery.","authors":"Hariharan Moorthy, Madhu Ramesh, Elumalai Premalatha, Thimmaiah Govindaraju","doi":"10.1039/d5mh01468a","DOIUrl":"https://doi.org/10.1039/d5mh01468a","url":null,"abstract":"<p><p>Dendrimer-based nucleic acid (NA) delivery systems have attracted significant attention due to their synthetic versatility, monodispersity, nuclease resistance, high payload release, and transfection efficiency. The conventional dendrimers are non-fluorescent, limiting their utility in real-time tracking and monitoring of drug delivery. Although terminal functionalization with fluorophores can partially address this issue, it often alters critical physicochemical properties and transfection efficiency. In this study, we report the design and development of far-red fluorescent dendrimers with a naphthalene diimide (NDI)-core for efficient and traceable gene and RNA delivery. These intrinsically fluorescent dendrimers enable real-time monitoring of cellular uptake and delivery. The NDI G3 formulation effectively condenses DNA, protects it from DNase-mediated degradation, and facilitates efficient transfection in cells. Therapeutically, NDI G3 demonstrated efficient glutathione peroxidase 4 (GPX4) siRNA delivery, comparable to PAMAM G3 and Lipofectamine 3000. Notably, the NDI G3-Ca<sup>2+</sup>-GPX4 siRNA-FINO2 formulation sensitizes human colon cancer-derived cells to ferroptosis, synergistically annihilating cancer cells compared to treatment with FINO2 alone. The intrinsically far-red fluorescent NDI G3 dendrimer with a dynamic fluorescence response developed for the combinatorial delivery of siRNA and drug molecules offers a generalized framework for designing next-generation far-red fluorescent dendrimers for nucleic acid therapeutics and theranostic applications.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766697","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
A desert locust-inspired wavelength-selective polarization vision system using two-dimensional ferroelectric heterostructures. 利用二维铁电异质结构的沙漠蝗虫波长选择偏振视觉系统。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01714a
Xiankai Lin, Qian Zhang, Wenbo Li, Fang Yi, Shihong Ma, Guitian Qiu, Jianxian Yi, Jiwei Chen, Yingjie Luo, Chunlei Zhang, Guigang Zhou, Ziling Chen, Qijie Liang

A bionic vision system integrates image sensing, memory, and computing capabilities, overcoming the limitations of traditional von Neumann architectures. However, integrating polarization-sensitivity and wavelength-selectivity while maintaining exceptional energy-efficiency, non-volatile and high-speed storage remains challenging for advanced application scenarios. Here, we present a bionic polarization vision system (BPVS) based on graphene (Gr)/CuInP2S6 (CIPS)/Gr/h-BN/PdSe2 (GCGhP) ferroelectric heterostructures, which achieves polarization-sensitive and wavelength-selective vision simulation. Optical excitation-induced ferroelectric polarization reversal confines the operational wavelength to the ultraviolet band. The anisotropy of PdSe2 introduces polarization sensitivity, while the ferroelectric polarization mechanism ensures ultra-low power consumption of 0.15 pJ/7.44 fJ (optical enhancement/electrical suppression per spike). The system mimics polarimetric synaptic plasticity and realizes memory imaging at multiple polarization angles. A bionic polarization vision neural network designed for polarization image demosaicking achieves super-resolution reconstruction. Our findings provide an effective pathway for advanced and energy-efficient polarization-sensitive bionic neuromorphic computing and vision systems.

仿生视觉系统集成了图像感知、记忆和计算能力,克服了传统冯·诺依曼架构的局限性。然而,在保持卓越的能效、非易失性和高速存储的同时,集成偏振灵敏度和波长选择性对于高级应用场景来说仍然是一个挑战。在此,我们提出了一种基于石墨烯(Gr)/CuInP2S6 (CIPS)/Gr/h-BN/PdSe2 (GCGhP)铁电异质结构的仿生极化视觉系统(bpv),该系统实现了极化敏感和波长选择性视觉模拟。光激发诱导的铁电极化反转将工作波长限制在紫外波段。PdSe2的各向异性引入了极化灵敏度,而铁电极化机制确保了超低功耗0.15 pJ/7.44 fJ(每尖峰光增强/电抑制)。该系统模拟极化突触可塑性,实现了多极化角度的记忆成像。设计了一种用于极化图像去马赛克的仿生极化视觉神经网络,实现了极化图像的超分辨率重建。我们的发现为先进和节能的极化敏感仿生神经形态计算和视觉系统提供了有效的途径。
{"title":"A desert locust-inspired wavelength-selective polarization vision system using two-dimensional ferroelectric heterostructures.","authors":"Xiankai Lin, Qian Zhang, Wenbo Li, Fang Yi, Shihong Ma, Guitian Qiu, Jianxian Yi, Jiwei Chen, Yingjie Luo, Chunlei Zhang, Guigang Zhou, Ziling Chen, Qijie Liang","doi":"10.1039/d5mh01714a","DOIUrl":"https://doi.org/10.1039/d5mh01714a","url":null,"abstract":"<p><p>A bionic vision system integrates image sensing, memory, and computing capabilities, overcoming the limitations of traditional von Neumann architectures. However, integrating polarization-sensitivity and wavelength-selectivity while maintaining exceptional energy-efficiency, non-volatile and high-speed storage remains challenging for advanced application scenarios. Here, we present a bionic polarization vision system (BPVS) based on graphene (Gr)/CuInP<sub>2</sub>S<sub>6</sub> (CIPS)/Gr/h-BN/PdSe<sub>2</sub> (GCGhP) ferroelectric heterostructures, which achieves polarization-sensitive and wavelength-selective vision simulation. Optical excitation-induced ferroelectric polarization reversal confines the operational wavelength to the ultraviolet band. The anisotropy of PdSe<sub>2</sub> introduces polarization sensitivity, while the ferroelectric polarization mechanism ensures ultra-low power consumption of 0.15 pJ/7.44 fJ (optical enhancement/electrical suppression per spike). The system mimics polarimetric synaptic plasticity and realizes memory imaging at multiple polarization angles. A bionic polarization vision neural network designed for polarization image demosaicking achieves super-resolution reconstruction. Our findings provide an effective pathway for advanced and energy-efficient polarization-sensitive bionic neuromorphic computing and vision systems.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Enhancing soft robots with chemical shielding for harsh corrosive liquid environments. 增强软机器人的化学防护,以适应恶劣的腐蚀性液体环境。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01593f
Haitao Qing, Sravanthi Vallabhuneni, Yinding Chi, Mohammad Javad Zarei, Pouya Sharbati, Haoze Sun, Jie Yin, Arun Kumar Kota

Soft robots offer safe interactions and adaptability for underwater applications such as environmental monitoring. However, their operation in corrosive liquid environments remains a challenge due to the degradation of elastomeric components upon exposure to acids, bases, and organic solvents. Here, a universal chemical shielding strategy is introduced for elastomer-based soft robots using a spray-coated superomniphobic skin composed of fluorinated silica nanoparticles. The coating exhibits high contact angles (>150°) and low roll-off angles (<10°) for liquids spanning a wide range of surface tensions, preventing wetting and protecting against strong acids and organic solvents. The strategy is applied to representative actuators made of silicone rubber, liquid crystal elastomers, and magnetic elastomer composites, actuated by pneumatic pressure, infrared light, and magnetic fields, respectively. These coated soft robots exhibit robust swimming, crawling, shape morphing, and manipulation without degradation under harsh chemical environments consisting of toluene, sulfuric acid, and chloroform. In contrast, uncoated counterparts suffer immediate and irreversible damage. This work establishes a scalable approach to chemically resilient soft robots capable of reliable operation in corrosive liquid environments, opening new possibilities for long-term deployment in biomedicine, chemical tank inspection, polluted water remediation, and offshore infrastructure maintenance.

软机器人为环境监测等水下应用提供了安全的交互和适应性。然而,由于弹性体组件暴露于酸、碱和有机溶剂中会降解,因此在腐蚀性液体环境中的操作仍然是一个挑战。本文介绍了一种通用的化学屏蔽策略,用于弹性体软机器人,该策略使用由氟化二氧化硅纳米颗粒组成的喷涂超疏水性皮肤。该涂层具有高接触角(约150°)和低滚脱角(约150°)。
{"title":"Enhancing soft robots with chemical shielding for harsh corrosive liquid environments.","authors":"Haitao Qing, Sravanthi Vallabhuneni, Yinding Chi, Mohammad Javad Zarei, Pouya Sharbati, Haoze Sun, Jie Yin, Arun Kumar Kota","doi":"10.1039/d5mh01593f","DOIUrl":"10.1039/d5mh01593f","url":null,"abstract":"<p><p>Soft robots offer safe interactions and adaptability for underwater applications such as environmental monitoring. However, their operation in corrosive liquid environments remains a challenge due to the degradation of elastomeric components upon exposure to acids, bases, and organic solvents. Here, a universal chemical shielding strategy is introduced for elastomer-based soft robots using a spray-coated superomniphobic skin composed of fluorinated silica nanoparticles. The coating exhibits high contact angles (>150°) and low roll-off angles (<10°) for liquids spanning a wide range of surface tensions, preventing wetting and protecting against strong acids and organic solvents. The strategy is applied to representative actuators made of silicone rubber, liquid crystal elastomers, and magnetic elastomer composites, actuated by pneumatic pressure, infrared light, and magnetic fields, respectively. These coated soft robots exhibit robust swimming, crawling, shape morphing, and manipulation without degradation under harsh chemical environments consisting of toluene, sulfuric acid, and chloroform. In contrast, uncoated counterparts suffer immediate and irreversible damage. This work establishes a scalable approach to chemically resilient soft robots capable of reliable operation in corrosive liquid environments, opening new possibilities for long-term deployment in biomedicine, chemical tank inspection, polluted water remediation, and offshore infrastructure maintenance.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12709453/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
A platform for the formation of uniform DNA condensate droplets using vibration-induced local vortices. 利用振动诱导的局部涡旋形成均匀DNA凝聚液滴的平台。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01304f
Zhitai Huang, Kanji Kaneko, Ryotaro Yoneyama, Tomoya Maruyama, Takeshi Hayakawa, Masahiro Takinoue, Hiroaki Suzuki

DNA condensate droplets (hereafter referred to as DNA condensates), which arise from specific interactions between sticky ends embedded in multi-arm DNA nanostructures, hold significant promise as programmable smart materials. However, from an engineering standpoint, the controlled preparation of DNA condensates with uniform size and a well-defined structure remains a major challenge due to the stochastic nature of the condensation process. This study presents a novel approach that employs vibration-induced local vortices (VILV) within a microfluidic platform to achieve spatial control over DNA condensate dimensions and enable their parallel generation. A key advantage of this platform is its ability to support direct observation and real-time tracking of structural morphology and dynamics. Through flow-field analysis of the VILV system, we demonstrate that uniform microvortices serve as semi-closed compartments, wherein DNA molecules confined within each vortex space rapidly aggregate and relax into uniform spherical condensate droplets. By modulating parameters such as DNA concentration and micropillar dimensions, the VILV platform not only enables systematic control of condensate size but also facilitates the construction of complex, multicomponent "patchy" condensates with consistent morphology. This platform provides a robust and scalable tool for studying liquid-liquid phase separation (LLPS) and offers broad potential for applications in the bottom-up synthesis of condensed molecular systems.

DNA凝聚液滴(以下简称DNA凝聚物)是由嵌入在多臂DNA纳米结构中的粘端之间的特定相互作用产生的,作为可编程智能材料具有重要的前景。然而,从工程的角度来看,由于冷凝过程的随机性,控制制备具有均匀尺寸和明确结构的DNA冷凝物仍然是一个主要挑战。本研究提出了一种新的方法,利用微流控平台内的振动诱导局部涡(VILV)来实现对DNA凝聚尺寸的空间控制,并使其平行产生。该平台的一个关键优势是它能够支持直接观察和实时跟踪结构形态和动力学。通过对VILV系统的流场分析,我们证明了均匀的微涡作为半封闭的隔室,被限制在每个涡旋空间内的DNA分子迅速聚集并松弛成均匀的球形冷凝液滴。通过调节DNA浓度和微柱尺寸等参数,VILV平台不仅可以系统地控制凝析物的大小,还可以促进构建具有一致形态的复杂、多组分“斑块”凝析物。该平台为研究液液相分离(LLPS)提供了一个强大且可扩展的工具,并在自下而上的缩合分子体系合成中提供了广泛的应用潜力。
{"title":"A platform for the formation of uniform DNA condensate droplets using vibration-induced local vortices.","authors":"Zhitai Huang, Kanji Kaneko, Ryotaro Yoneyama, Tomoya Maruyama, Takeshi Hayakawa, Masahiro Takinoue, Hiroaki Suzuki","doi":"10.1039/d5mh01304f","DOIUrl":"https://doi.org/10.1039/d5mh01304f","url":null,"abstract":"<p><p>DNA condensate droplets (hereafter referred to as DNA condensates), which arise from specific interactions between sticky ends embedded in multi-arm DNA nanostructures, hold significant promise as programmable smart materials. However, from an engineering standpoint, the controlled preparation of DNA condensates with uniform size and a well-defined structure remains a major challenge due to the stochastic nature of the condensation process. This study presents a novel approach that employs vibration-induced local vortices (VILV) within a microfluidic platform to achieve spatial control over DNA condensate dimensions and enable their parallel generation. A key advantage of this platform is its ability to support direct observation and real-time tracking of structural morphology and dynamics. Through flow-field analysis of the VILV system, we demonstrate that uniform microvortices serve as semi-closed compartments, wherein DNA molecules confined within each vortex space rapidly aggregate and relax into uniform spherical condensate droplets. By modulating parameters such as DNA concentration and micropillar dimensions, the VILV platform not only enables systematic control of condensate size but also facilitates the construction of complex, multicomponent \"patchy\" condensates with consistent morphology. This platform provides a robust and scalable tool for studying liquid-liquid phase separation (LLPS) and offers broad potential for applications in the bottom-up synthesis of condensed molecular systems.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
The dark matter in water, air and land: from microplastic to invisible nanoplastics. 水、空气和土地中的暗物质:从微塑料到不可见的纳米塑料。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/d5mh01544h
Martina H Stenzel

Microplastic is well known and has been the subject of many review articles. In recent years, an increasing number of reports have documented the presence of nanoplastics-plastic particles smaller than 1 µm-in various environments, from the ocean to the human brain. In this article, I focus on nanoparticles and what we do and do not understand about their effects on our health. After an introduction to nanoplastics and their size relative to a single polymer chain, the degradation process that produces nanoplastics, similar to microplastics, is briefly summarized. Due to their high surface area, nanoplastics can behave differently in solution because they tend to aggregate. After reviewing the presence of microplastics and nanoplastics in humans, insights from the established field of nanomedicine are used to explore how nanoplastics may enter the bloodstream and reach the brain. This also includes the topic of protein corona formation, which influences the fate of nanoplastics in the body. Finally, a brief summary on the impact of plastic particles on health is provided, focusing on reports comparing nano- and microplastics. This article concludes with how materials scientists and chemists can contribute to addressing the rising plastic pollution problem.

微塑料是众所周知的,已经成为许多评论文章的主题。近年来,越来越多的报告记录了纳米塑料(小于1微米的塑料颗粒)在各种环境中的存在,从海洋到人脑。在这篇文章中,我将重点关注纳米颗粒,以及我们对它们对我们健康的影响的了解和不了解。在介绍了纳米塑料及其相对于单个聚合物链的尺寸之后,简要总结了产生纳米塑料的降解过程,类似于微塑料。由于它们的高表面积,纳米塑料在溶液中表现不同,因为它们倾向于聚集。在回顾了微塑料和纳米塑料在人体中的存在之后,纳米医学领域的见解被用于探索纳米塑料如何进入血液并到达大脑。这也包括蛋白质电晕形成的主题,它影响纳米塑料在体内的命运。最后,简要总结了塑料颗粒对健康的影响,重点介绍了比较纳米塑料和微塑料的报告。这篇文章总结了材料科学家和化学家如何为解决日益严重的塑料污染问题做出贡献。
{"title":"The dark matter in water, air and land: from microplastic to invisible nanoplastics.","authors":"Martina H Stenzel","doi":"10.1039/d5mh01544h","DOIUrl":"https://doi.org/10.1039/d5mh01544h","url":null,"abstract":"<p><p>Microplastic is well known and has been the subject of many review articles. In recent years, an increasing number of reports have documented the presence of nanoplastics-plastic particles smaller than 1 µm-in various environments, from the ocean to the human brain. In this article, I focus on nanoparticles and what we do and do not understand about their effects on our health. After an introduction to nanoplastics and their size relative to a single polymer chain, the degradation process that produces nanoplastics, similar to microplastics, is briefly summarized. Due to their high surface area, nanoplastics can behave differently in solution because they tend to aggregate. After reviewing the presence of microplastics and nanoplastics in humans, insights from the established field of nanomedicine are used to explore how nanoplastics may enter the bloodstream and reach the brain. This also includes the topic of protein corona formation, which influences the fate of nanoplastics in the body. Finally, a brief summary on the impact of plastic particles on health is provided, focusing on reports comparing nano- and microplastics. This article concludes with how materials scientists and chemists can contribute to addressing the rising plastic pollution problem.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" ","pages":""},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145766720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Microenvironments between cathode active materials and solid electrolytes for all-solid-state batteries 全固态电池正极活性材料与固体电解质之间的微环境。
IF 10.7 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-12-17 DOI: 10.1039/D5MH02003D
Ju-Hyeon Lee, Eun Seo Kang, Ji Young Kim, Ki Yoon Bae and Ji Hoon Lee

All-solid-state batteries (ASSBs) are promising next-generation energy storage systems; however, their performance is often constrained by poorly understood interfacial phenomena within composite cathode (CC) layers. In this study, we systematically elucidate how the microenvironment of CC layers, controlled by the mixing sequence of cathode active material (CAM), solid electrolyte (SE), and conductive carbon, determines the electrochemical performance of ASSBs. By preparing three representative CC configurations, we demonstrate that uniform CAM|SE interfaces promote well-developed lithium-ion transport pathways, leading to enhanced rate capability and long-term cycling stability. In contrast, poor CAM|SE contact increases charge-transfer resistance and results in premature cell failure within tens of cycles. Multiscale synchrotron-based characterizations reveal the mechanistic origin of this performance disparity. Interfacial inhomogeneity induces particle-level state-of-charge heterogeneity, which leads to localized CAM overcharging and subsequent SE decomposition. The significance of uniform CAM|SE interfaces becomes even more pronounced under practical conditions. At 30 °C, where ionic transport is intrinsically limited, ASSB cells with uniform CAM|SE interfaces maintain stable cycling performance, whereas those with less-uniform interfaces fail at an early stage. Finally, pouch-type anodeless ASSB cells operated under low stack pressure reproduce the same performance trends, further underscoring the critical role of CC microstructure control. Overall, this work establishes a direct correlation between CAM|SE interfacial uniformity, SE stability, and ASSB performance, providing practical guidelines for engineering reproducible, high-performance CC layers that bridge laboratory-scale demonstrations with real-world applications.

全固态电池(assb)是很有前途的下一代储能系统;然而,它们的性能往往受到复合阴极(CC)层内界面现象的限制。在这项研究中,我们系统地阐明了在阴极活性物质(CAM)、固体电解质(SE)和导电碳的混合顺序控制下,CC层的微环境如何决定assb的电化学性能。通过制备三种具有代表性的CC配置,我们证明了均匀的CAM|SE界面促进了良好的锂离子传输途径,从而提高了速率能力和长期循环稳定性。相反,不良的CAM|SE接触会增加电荷转移阻力,并导致数十个周期内细胞过早衰竭。基于多尺度同步加速器的表征揭示了这种性能差异的机理根源。界面的不均匀性导致粒子级电荷状态的不均匀性,导致局部CAM过充和随后的SE分解。在实际条件下,均匀的CAM|SE界面的意义更加明显。在30°C下,离子传输本质上受到限制,具有均匀CAM|SE界面的ASSB电池保持稳定的循环性能,而那些界面不均匀的ASSB电池在早期阶段失效。最后,在低堆压下工作的袋型无阳极ASSB电池重现了相同的性能趋势,进一步强调了CC微观结构控制的关键作用。总的来说,这项工作建立了CAM|SE界面均匀性、SE稳定性和ASSB性能之间的直接相关性,为工程可复制、高性能CC层提供了实用指南,将实验室规模的演示与实际应用联系起来。
{"title":"Microenvironments between cathode active materials and solid electrolytes for all-solid-state batteries","authors":"Ju-Hyeon Lee, Eun Seo Kang, Ji Young Kim, Ki Yoon Bae and Ji Hoon Lee","doi":"10.1039/D5MH02003D","DOIUrl":"10.1039/D5MH02003D","url":null,"abstract":"<p >All-solid-state batteries (ASSBs) are promising next-generation energy storage systems; however, their performance is often constrained by poorly understood interfacial phenomena within composite cathode (CC) layers. In this study, we systematically elucidate how the microenvironment of CC layers, controlled by the mixing sequence of cathode active material (CAM), solid electrolyte (SE), and conductive carbon, determines the electrochemical performance of ASSBs. By preparing three representative CC configurations, we demonstrate that uniform CAM|SE interfaces promote well-developed lithium-ion transport pathways, leading to enhanced rate capability and long-term cycling stability. In contrast, poor CAM|SE contact increases charge-transfer resistance and results in premature cell failure within tens of cycles. Multiscale synchrotron-based characterizations reveal the mechanistic origin of this performance disparity. Interfacial inhomogeneity induces particle-level state-of-charge heterogeneity, which leads to localized CAM overcharging and subsequent SE decomposition. The significance of uniform CAM|SE interfaces becomes even more pronounced under practical conditions. At 30 °C, where ionic transport is intrinsically limited, ASSB cells with uniform CAM|SE interfaces maintain stable cycling performance, whereas those with less-uniform interfaces fail at an early stage. Finally, pouch-type anodeless ASSB cells operated under low stack pressure reproduce the same performance trends, further underscoring the critical role of CC microstructure control. Overall, this work establishes a direct correlation between CAM|SE interfacial uniformity, SE stability, and ASSB performance, providing practical guidelines for engineering reproducible, high-performance CC layers that bridge laboratory-scale demonstrations with real-world applications.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" 2","pages":" 736-747"},"PeriodicalIF":10.7,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145809009","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
期刊
Materials Horizons
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1