Materials Today最新文献_第7页

International perspectives on glass waste form development for low-level and intermediate-level radioactive waste 低放射性和中放射性废物玻璃废物形式发展的国际视角

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.08.025

John S. McCloy , Brian J. Riley , Malin C. Dixon Wilkins , Jonathan S. Evarts , John Bussey , John D. Vienna , Paul A. Bingham , Daniel J. Gregg , Michael Ojovan , Sophie Schuller , Kazuyoshi Uruga , Damien Perret , Elise Regnier , Isabelle Giboire , Wooyong Um , Kai Xu , Ashutosh Goel , Albert A. Kruger

The global transition to low-carbon energy sources will require a significant contribution of nuclear energy to achieve emission goals. Low-level radioactive wastes (LLW) and intermediate-level radioactive wastes (ILW) are created in various phases of the nuclear fuel cycle for power generation, as well as from nuclear accidents, legacy weapons production, contaminated site decommissioning, and other nuclear activities such as radiopharmaceutical production. In this review, we will summarize recent developments, state-of-the-art glass formulations, and thermal treatment process developments for vitrification of nuclear LLW and ILW from programs in Europe, Asia, Australia, and North America. Throughout, we will discuss the selection of glass over other possible waste forms and any special processing considerations due to the nature of the waste. The characteristics of the wastes, such as mixed technological waste, waste coming from dismantling of reprocessing facilities, site decommissioning, and accident site decontamination, are important considerations. This is balanced with the suite of technologies available to vitrify these wastes, e.g., variations of incineration, in-can melting, and plasma treatment. Glass properties and microstructural aspects are compared to give an overview of the versatility of packaging matrices, such as homogeneous glasses, composites, and crystalline matrices. The volume and heterogeneity of the waste, specific radionuclide content, and solubility of components in silicate melts, all factor into the selection of a given waste form, processing route, and technology. Case studies include examples from the United States, United Kingdom, the Russian Federation, France, Australia, Japan, Korea, and China.

全球向低碳能源过渡需要核能为实现排放目标做出重大贡献。低放射性废物（LLW）和中放射性废物（ILW）产生于核燃料循环发电的各个阶段，以及核事故、遗留武器生产、污染场地退役和放射性药物生产等其他核活动。在本综述中，我们将总结欧洲、亚洲、澳大利亚和北美在核低放废物和间接放射性废物玻璃化方面的最新进展、最先进的玻璃配方以及热处理工艺的发展。在整个过程中，我们将讨论选择玻璃而非其他可能的废物形式，以及因废物性质而产生的任何特殊处理考虑因素。废弃物的特性，如混合技术废弃物、后处理设施拆除产生的废弃物、场地退役和事故现场去污等，都是重要的考虑因素。这需要与可用于这些废物玻璃化的一系列技术相平衡，例如各种焚烧、罐内熔化和等离子处理技术。通过对玻璃特性和微观结构方面的比较，可以了解包装基质（如均质玻璃、复合材料和结晶基质）的多功能性。废物的体积和异质性、特定放射性核素含量以及硅酸盐熔体中成分的溶解度，都是选择特定废物形式、处理路线和技术的因素。案例研究包括来自美国、英国、俄罗斯联邦、法国、澳大利亚、日本、韩国和中国的实例。

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引用次数: 0

Advanced anti-ablation C/C composites: structural design strategies and future perspective 先进的抗烧蚀碳/碳复合材料：结构设计策略与未来展望

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.004

Xin Zhang , Lingjun Guo , Huimin Liu , Yulei Zhang , Qiangang Fu , Xuemin Yin , Hejun Li

Carbon fiber reinforced carbon matrix (carbon/carbon, C/C) composites are promising thermal protection candidates for ultra-high temperature applications. However, their high oxidation sensitivity poses a use limitation in ultra-high temperature and high-speed aerobic environments. Matrix modification and coating technology with Si-based or ultra-high temperature ceramics have proved to be highly effective in improving the oxidation and ablation resistance of C/C composites. Nevertheless, challenges persist due to the inherent brittleness and poor thermal conductivity of ceramics, the inability of modified C/C composites to form dense oxide barrier layers, and thermo-physical mismatch issues that lead to crack formation and coating falloff. Thus, the development of high-performance C/C composites is ongoing and a series of advancements have been achieved, focusing on alleviating local overheating and insufficient ablation resistance, while also enhancing the component structural stability. To expedite the development of anti-ablation C/C composites and avoid aimless trial-and-error efforts, this review comprehensively summarizes the latest significant progress and breakthroughs achieved in the area. A brief overview of the structure, fabrication methods and ablation testing techniques of C/C composites is first introduced. The following emphasis is on discussing different structural design strategies on carbon fibers, preforms, matrix carbon, modification and coating methods, aiming to provide insightful design principles and valuable references for future research activities. Finally, the ongoing challenges and research directions in the future of developing high-performance anti-ablation C/C composites, incorporating our insights and perspectives, are discussed.

碳纤维增强碳基（碳/碳，C/C）复合材料在超高温应用中是很有前途的热保护材料。然而，它们的高氧化敏感性限制了它们在超高温和高速有氧环境中的应用。事实证明，使用硅基或超高温陶瓷进行基体改性和涂层技术可有效提高碳/碳复合材料的抗氧化性和抗烧蚀性。然而，由于陶瓷固有的脆性和较差的导热性、改性 C/C 复合材料无法形成致密的氧化物阻挡层，以及热物理不匹配问题导致裂纹形成和涂层脱落，这些挑战依然存在。因此，高性能 C/C 复合材料的开发工作一直在进行，并取得了一系列进展，重点是缓解局部过热和抗烧蚀能力不足的问题，同时还能增强部件结构的稳定性。为了加快抗烧蚀 C/C 复合材料的开发，避免漫无目的的试错，本综述全面总结了该领域取得的最新重大进展和突破。首先简要介绍了 C/C 复合材料的结构、制造方法和烧蚀测试技术。接下来重点讨论了碳纤维、预制件、基质碳、改性和涂层方法等不同的结构设计策略，旨在为未来的研究活动提供有见地的设计原则和有价值的参考。最后，结合我们的见解和观点，讨论了未来开发高性能抗烧蚀碳/碳复合材料所面临的挑战和研究方向。

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引用次数: 0

A bioorthogonal probiotic platform spatiotemporally releases nanobodies in deep tumor for cancer chemoimmunotherapy 生物正交益生菌平台在肿瘤深部时空释放纳米抗体，用于癌症化疗免疫疗法

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.002

Ruiyue Chen , Qianglan Lu , Fei Zeng , Shurong Qin , Yongchun Pan , Zhiyong Liu , Yuzhen Wang , Bangshun He , Wenjin Qi , Yujun Song

The effectiveness of immune checkpoint blockade therapies in treating solid tumors is hindered by the limited activation of the tumor immune microenvironment within deep tumors. Immunogenic cell death offers a promising method to enhance anti-tumor immune responses. Integrating these two approaches in cancer chemoimmunotherapy presents a novel perspective. Here, a self-mineralized bioorthogonal probiotic platform with the expression of anti-PD-L1 nanobodies was developed for cancer chemoimmunotherapy. This platform selectively accumulated and deeply penetrated into tumor tissues, where the palladium-mineralized probiotics catalyzed bioorthogonal bond-cleavage to generate chemotherapeutic drugs and induced immunogenic cell death. Under laser irradiation, the indocyanine green modified probiotics were ruptured and released nanobodies which effectively suppressed tumor immune evasion and ultimately led to the tumor-specific immune responses. This innovative platform resulted in significant inhibition of tumor growth and lung metastasis. Overall, these findings suggest that synergistically enhancing antitumor immunity through the induction of immunogenic cell death via bioorthogonality and PD-L1 blocking as a therapeutic strategy could improve cancer chemoimmunotherapy.

免疫检查点阻断疗法治疗实体瘤的有效性受到深部肿瘤内肿瘤免疫微环境激活有限的阻碍。免疫性细胞死亡为增强抗肿瘤免疫反应提供了一种前景广阔的方法。在癌症化学免疫疗法中整合这两种方法提出了一个新的视角。在此，我们开发了一种表达抗PD-L1纳米抗体的自矿化生物正交益生菌平台，用于癌症化疗免疫疗法。该平台可选择性地积聚并深入肿瘤组织，钯矿化益生菌在其中催化生物正交键裂解生成化疗药物，并诱导免疫性细胞死亡。在激光照射下，吲哚菁绿修饰的益生菌破裂并释放出纳米抗体，从而有效抑制肿瘤免疫逃避，并最终导致肿瘤特异性免疫反应。这一创新平台显著抑制了肿瘤生长和肺转移。总之，这些研究结果表明，通过生物正交性诱导免疫原性细胞死亡和 PD-L1 阻断作为一种治疗策略，协同增强抗肿瘤免疫，可以改善癌症化疗免疫疗法。

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引用次数: 0

On the mechanistic origin of nanoscale “cold welding” 纳米级 "冷焊接 "的机理起源

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.013

Peng Dong , Bo Song , Xin Zhai , Yanfei Gao

When nano-objects are brought together into contacts without any applied load at or near room temperature, a solid-state bonding can be accomplished either instantaneously or within some time, which has been termed by many recent works as “cold welding” as opposed to the traditional fusion welding. Such phenomena are more often encountered at nanoscale and have been utilized to build nano-devices such as nanowire-based interconnects or electrodes. Clearly, cold welding could be merely driven by the elastic adhesive contact, the analysis of which is straightforward but does not involve a time dependence. Room temperature, nanoscale, and contact size growth might suggest the operation of the curvature-driven sintering mechanism, or result from our proposed interfacial diffusional process in this paper as driven by a stress gradient (i.e., Coble creep). Here, we fabricated silver nanowires (AgNWs) with radius of several tens of nanometers, placed them into interconnect-like contacts, and measured the contact size growth at selected temperatures up to 200 °C. Out of the two hypothetical mechanisms (sintering versus Coble), only the latter mechanism can compare favorably with our experiments and result into physically meaningful parameters such as the activation energy and stress gradient magnitude. Consequently, this work presents the first conclusive study for nanoscale cold welding, as being the Coble diffusional creep.

当纳米物体在室温或接近室温的条件下接触而没有任何外加载荷时，可以瞬间或在一段时间内完成固态结合，与传统的熔焊相比，最近的许多研究将其称为 "冷焊"。这种现象在纳米尺度上更为常见，并被用于制造纳米器件，如基于纳米线的互连器件或电极。显然，冷焊可能仅仅是由弹性粘合剂接触驱动的，其分析简单明了，但不涉及时间依赖性。室温、纳米尺度和接触尺寸的增长可能表明曲率驱动烧结机制的运行，或者是我们在本文中提出的应力梯度（即 Coble 蠕变）驱动的界面扩散过程的结果。在这里，我们制作了半径为几十纳米的银纳米线（AgNWs），将其放入类似互连的接触中，并在选定的温度（最高达 200 °C）下测量了接触尺寸的增长。在两种假设机制（烧结和 Coble）中，只有后一种机制能与我们的实验相比较，并得出有物理意义的参数，如活化能和应力梯度大小。因此，这项工作首次提出了纳米级冷焊接的结论性研究，即 Coble 扩散蠕变。

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引用次数: 0

On the role of charge transfer excitations in non-fullerene acceptors for organic photovoltaics 非富勒烯有机光伏受体中电荷转移激发的作用

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.009

Samuele Giannini , Daniel J.C. Sowood , Jesús Cerdá , Siebe Frederix , Jeannine Grüne , Giacomo Londi , Thomas Marsh , Pratyush Ghosh , Ivan Duchemin , Neil C. Greenham , Koen Vandewal , Gabriele D’Avino , Alexander J. Gillett , David Beljonne

Through the development of new non-fullerene electron acceptor (NFA) materials, such as Y6 and its molecular derivatives, the power conversion efficiencies of organic photovoltaics (OPVs) have now exceeded 19 %. However, despite this rapid progress, our fundamental understanding of the unique optical and electronic properties of these Y-series NFAs is lacking, and this currently limits progress in material design. In this work, we provide a detailed computational-experimental characterisation of the archetypal NFA, Y6. To explain the significant broadening and red shift of the absorption spectrum observed when moving from the solution phase to the solid state, we first rule out more typical causes, such as J-aggregation. Instead, by considering the role of charge transfer (CT) excitations and their mixing with Frenkel exciton (FE) states, we can computationally reproduce the experimental absorption spectra of Y6 with excellent accuracy. Using transient absorption spectroscopy, we provide evidence for this dense manifold of FE-CT hybrid electronic excitations in Y6 through the prominent sub-picosecond relaxation events following supra band gap excitation. Furthermore, through sub band gap excitation, we also find states with polaronic character in Y6 that are in a dynamic equilibrium with the FE-CT hybrid states. Magnetic resonance spectroscopies reveal that these polaronic states are polaron pairs, most likely located on neighbouring Y6 molecules, not free charge carriers, as has been previously suggested. Thus, this new understanding of how the solid-state packing motif directly controls the optical and electronic properties of Y-series NFAs opens the door to intelligently design NFA materials to further increase OPV performance.

通过开发 Y6 及其分子衍生物等新型非富勒烯电子受体 (NFA) 材料，有机光伏 (OPV) 的功率转换效率现已超过 19%。然而，尽管取得了如此快速的进展，我们对这些 Y 系列 NFA 独特的光学和电子特性仍缺乏基本的了解，这也限制了材料设计的进展。在这项工作中，我们对 Y6 这种典型的 NFA 进行了详细的计算-实验表征。为了解释从溶液相转变到固态时观察到的吸收光谱的显著拓宽和红移，我们首先排除了更典型的原因，如 J 聚集。相反，通过考虑电荷转移（CT）激发的作用及其与弗伦克尔激子（FE）态的混合，我们可以通过计算非常准确地再现 Y6 的实验吸收光谱。利用瞬态吸收光谱，我们通过超带隙激发后显著的亚皮秒弛豫事件，为 Y6 中 FE-CT 混合电子激发的密集流形提供了证据。此外，通过亚带隙激发，我们还在 Y6 中发现了与 FE-CT 混合态处于动态平衡的极性态。磁共振光谱显示，这些极性态是极子对，很可能位于相邻的 Y6 分子上，而不是以前认为的自由电荷载流子。因此，对固态填料结构如何直接控制 Y 系列非氟化碳的光学和电子特性的这一新认识，为智能设计非氟化碳材料以进一步提高 OPV 性能打开了大门。

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引用次数: 0

Advanced design of high-performance artificial neuromorphic electronics 高性能人工神经形态电子学的高级设计

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.08.027

Ying Cao , Hong Fu , Xi Fan , Xiaocong Tian , Jingxin Zhao , Jian Lu , Zhen Liang , Bingang Xu

Recent years have witnessed the significant progress of nature artificial neuromorphic systems with advances achieved in interdisciplinary fields, like neurosciences, electronics and materials science. The research with focus on learning from human has been conducted from various hierarchy, aiming to realize the intelligent way of human to process information to the largest extent. Significant advancement in artificial neuromorphic electronics has been realized recently, like the ultrasmall size fabrication and high‐density integration of organic synapse. Though a few reviews presented the development from certain aspect, review in the view of the comprehensive learning from human at all levels, ranging from morphologies, structures, distributions of the device arrays and the computing mode of the brain, to fully simulate the function of human, is lacking. Here, the new developments are timely and systematically reviewed for advanced design of high-performance nature artificial neuromorphic electronics. First, recent breakthrough and mechanisms are illustrated, and then the elaborated considerations for the components of artificial neuromorphic devices are demonstrated based on perspective of learning from human neuromorphic systems from various hierarchy. After that, strategies are summarized to enhance the overall performance of the systems by taking the whole information processing procedure into consideration, and then the design thought for future artificial neuromorphic electronics is proposed. Finally, some perspectives are put forward.

近年来，随着神经科学、电子学和材料科学等跨学科领域取得的进展，自然界人工神经形态系统取得了重大进展。以向人类学习为重点的研究已从不同层次展开，旨在最大程度地实现人类处理信息的智能方式。最近，人工神经形态电子学取得了重大进展，如超小型制造和高密度集成有机突触。虽然有一些综述从某些方面介绍了这一发展，但缺乏从形态、结构、器件阵列分布和大脑计算模式等各个层面全面学习人类，以完全模拟人类功能的综述。在此，我们将及时、系统地评述这些新进展，以促进高性能人工神经形态电子学的先进设计。首先，阐述了最近的突破和机制，然后基于从不同层次学习人类神经形态系统的视角，详细论证了人工神经形态设备组件的注意事项。随后，从整个信息处理过程出发，总结了提高系统整体性能的策略，并提出了未来人工神经形态电子设备的设计思路。最后，提出了一些展望。

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引用次数: 0

Omnidirectional elastic constraint-based embedded 3D printing in non-yield stress fluids for engineering complex tissues 在非屈服应力流体中基于全向弹性约束的嵌入式 3D 打印，用于复杂组织的工程设计

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.08.005

Bingyan Wu , Zhaoxi Zeng , Yongcong Fang , Zhenrui Zhang , Yueming Tian , Bingchuan Lu , Binhan Li , Zibo Liu , Ting Zhang , Zhuo Xiong

Embedded 3D printing, relying on yield-stress fluid-based supporting baths, has significantly expanded our ability to create complex tissues and organs. However, many extracellular matrix-based hydrogels, despite their excellent biological performance, such as gelatin and hyaluronic acid (HA) hydrogels, lack yield-stress properties, limiting their use in embedded 3D printing and hindering functional maturation of complex tissue constructs. To address this challenge, we present a method for embedded printing in non-yield stress fluids using sequential printing in a reversible ink template (SPIRIT) strategy. By leveraging an omnidirectional elastic constraint provided by conventional supporting baths, we can precisely fabricate GelMA and HAMA hydrogels into functional tissue constructs with both intricate external structures and internal vessel systems, which cannot be achieved with extant embedded printing techniques. As a proof of concept, we successfully printed a complex ventricle model with high cell density and internal channels using GelMA hydrogel, which demonstrated high cell viability and synchronous beating performance. The omnidirectional elastic constraint-based SPIRIT technique holds promise for advancing organ printing with remarkable structural complexities and biomaterials affinity akin to natural tissue constructs by decoupling from yield-stress fluids.

嵌入式三维打印依靠屈服应力流体支撑浴，大大提高了我们创建复杂组织和器官的能力。然而，许多基于细胞外基质的水凝胶（如明胶和透明质酸（HA）水凝胶）尽管具有出色的生物学性能，但却缺乏屈服应力特性，这限制了它们在嵌入式三维打印中的应用，并阻碍了复杂组织构建物的功能成熟。为了应对这一挑战，我们提出了一种在非屈服应力流体中使用可逆油墨模板顺序打印（SPIRIT）策略进行嵌入打印的方法。通过利用传统支撑浴提供的全向弹性约束，我们可以精确地将 GelMA 和 HAMA 水凝胶制造成具有复杂外部结构和内部血管系统的功能性组织构建体，这是现有嵌入式打印技术无法实现的。作为概念验证，我们使用 GelMA 水凝胶成功打印出了一个具有高细胞密度和内部通道的复杂心室模型，该模型显示出很高的细胞存活率和同步跳动性能。基于全向弹性约束的SPIRIT技术有望推动器官打印技术的发展，通过与屈服应力流体脱钩，使器官具有显著的结构复杂性和与天然组织结构相似的生物材料亲和性。

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引用次数: 0

Cooperative effect of complementary antisense oligonucleotides and CRISPR effectors for universal DNA-based pathogen assay using nano-enabled colorimetry 互补反义寡核苷酸和 CRISPR 效应器的协同效应，利用纳米比色法进行基于 DNA 的通用病原体检测

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.017

Ketan Dighe , Parikshit Moitra , Pranay Saha , Nivetha Gunaseelan , Dipanjan Pan

Infectious diseases continue to pose significant challenges to global health, necessitating the development of diagnostic methodologies that are not only rapid and precise but also universally accessible. Herein, we developed a colorimetric CRISPR-Cas12a assay that utilizes CRISPR gene-editing technology, gold nanoparticles (AuNPs), and DNA hybridization principles to target a range of antibiotic-resistant and emerging pathogens, including Chlamydia trachomatis (CT), Neisseria gonorrhoeae (NG), Candida auris (CA), and Human Papillomavirus (HPV). The assay utilizes specially engineered CRISPR-RNA (crRNA) and single-stranded oligonucleotides (ssDNAs) that correspond to a complementary single-stranded DNA sequence, termed the ’linker probe,’ which targets conserved genetic regions to enhance specificity and sensitivity. This design facilitates a simple visual readout through significant changes in the optical properties of AuNPs when the Cas12a enzyme, activated by target DNA, cleaves the linker probe. The assay, which does not require DNA amplification, demonstrated the ability to detect these pathogens with a detection limit of 7–8 copies/µL and achieved a clinical sensitivity of 100 % in detecting Chlamydia trachomatis and Neisseria gonorrhoeae from 60 de-identified clinical samples. Additionally, it directly detects DNA from these pathogens without the need for DNA extraction, employing a multiplexed lateral flow-based platform suitable for rapid clinical monitoring. This novel diagnostic approach offers significant improvements in the detection and management of infectious diseases, particularly in resource-limited settings, due to its simplicity, cost-effectiveness, and high specificity and sensitivity.

传染病继续对全球健康构成重大挑战，因此有必要开发不仅快速、精确而且普遍可用的诊断方法。在此，我们开发了一种比色 CRISPR-Cas12a 检测方法，利用 CRISPR 基因编辑技术、金纳米粒子 (AuNPs) 和 DNA 杂交原理，靶向一系列抗生素耐药和新出现的病原体，包括沙眼衣原体 (CT)、淋病奈瑟菌 (NG)、白色念珠菌 (CA) 和人类乳头瘤病毒 (HPV)。该检测方法利用专门设计的 CRISPR-RNA (crRNA) 和单链寡核苷酸 (ssDNA)，这些寡核苷酸与互补的单链 DNA 序列（称为 "连接探针"）相对应，以保守的基因区域为目标，从而提高了特异性和灵敏度。当 Cas12a 酶被目标 DNA 激活并裂解连接体探针时，AuNPs 的光学特性会发生显著变化，这种设计有助于通过简单的视觉读数进行分析。该检测方法无需进行 DNA 扩增，就能检测出这些病原体，检测限为 7-8 个拷贝/微升，在检测 60 份去标识临床样本中的沙眼衣原体和淋病奈瑟菌时，临床灵敏度达到 100%。此外，它还能直接检测这些病原体的 DNA，无需进行 DNA 提取，采用的是基于侧向流的多路复用平台，适用于快速临床监测。这种新型诊断方法因其简便、成本效益高、特异性和灵敏度高，大大改善了传染病的检测和管理，尤其是在资源有限的环境中。

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引用次数: 0

Ferroelectric interface for efficient sodium metal cycling in anode-free solid-state batteries 用于无阳极固态电池中金属钠高效循环的铁电界面

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.018

Chen Sun , Yang Li , Zheng Sun , Xuanyi Yuan , Haibo Jin , Yongjie Zhao

Anode-free solid-state batteries (AFSSBs) are considered one of the promising solutions for achieving high energy density and safety of electrochemical energy storage systems. However, owing to mechanochemical contact losses and metallic dendrite growth caused by the degradation at the current collector (CC)/electrolyte interface, the feasibility of AFSSBs is critically limited, especially upon the involvement of rigid ceramic electrolytes. Here, a new strategy is reported for NASICON-structure Na₃Zr₂Si₂PO₁₂ (NZSP) electrolyte-based AFSSBs by introducing a resilient ferroelectric composite substrate coated onto Al CC, eventually achieving efficient and stable operation. Compared with the bare Al foil, the ferroelectric composite substrate not only renders an intimate CC/electrolyte interface compatibility, but also dynamically regulates the distribution and migration of Na⁺ flux at the CC/electrolyte interface through the built-in electric field stem from ferroelectric BaTiO₃, guiding homogeneous and dense sodium metal deposition. Stable plating/stripping cycling can be achieved even at a high current density of 1.2mA cm⁻² with the Coulombic efficiency of (99.7 %). Significantly, the NZSP-based AFSSB integrated with the ferroelectric composite substrate and mainstream sodium ion cathodes demonstrates stable cycling and excellent capacity retention.

无阳极固态电池（AFSSB）被认为是实现电化学储能系统高能量密度和安全性的理想解决方案之一。然而，由于集流体（CC）/电解质界面降解引起的机械化学接触损失和金属枝晶生长，AFSSB 的可行性受到严重限制，尤其是在使用刚性陶瓷电解质时。本文报告了一种基于 NASICON 结构的 Na3Zr2Si2PO12（NZSP）电解质的 AFSSB 的新策略，即在 Al CC 上涂覆弹性铁电复合基底，最终实现高效稳定的运行。与裸铝箔相比，铁电复合基底不仅能使 CC 与电解质界面紧密兼容，还能通过铁电 BaTiO3 的内置电场干系动态调节 Na+ 通量在 CC 与电解质界面的分布和迁移，引导金属钠均匀致密地沉积。即使在 1.2mA cm-2 的高电流密度下，也能实现稳定的电镀/剥离循环，库仑效率高达（99.7%）。值得注意的是，基于 NZSP 的 AFSSB 集成了铁电复合基底和主流钠离子阴极，可实现稳定的循环和出色的容量保持。

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引用次数: 0

Unsupervised physics-informed disentanglement of multimodal materials data 多模态材料数据的无监督物理信息解缠

IF 21.1 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Today

Pub Date : 2024-11-01 DOI: 10.1016/j.mattod.2024.09.005

Nathaniel Trask , Carianne Martinez , Troy Shilt , Elise Walker , Kookjin Lee , Anthony Garland , David P. Adams , John F. Curry , Michael T. Dugger , Steven R. Larson , Brad L. Boyce

Materials, and the processes used in their synthesis, are commonly evaluated via a variety of experimental modalities, each individually describing some aspect of the process conditions, material structure, chemistry, material properties, and associated performance. Traditionally, materials experts are called upon to make sense of this collage of disparate information. However, emerging algorithms offer an opportunity to fuse these complementary measurements from multiple distinct modalities into a holistic, high-dimensional descriptor of the material state. We present herein a probabilistic framework for discovering such shared information in multimodal datasets. Through an unsupervised approach based on variational inference, we identify semantic clusters that encode correlation across modalities, thereby obtaining physically meaningful fingerprints that indicate distinct mechanistic regimes of performance. This multimodality can be further enriched through the incorporation of physics-based constitutive models that can facilitate cluster disentanglement. The probabilistic underpinnings of the approach provide uncertainty quantification to evaluate reliability of cross-modal estimation and quantify how individual modalities contribute more than the sum of their parts. The approach is demonstrated for a collection of three multimodal datasets related to material reliability.

材料及其合成工艺通常通过各种实验方式进行评估，每种方式都单独描述了工艺条件、材料结构、化学性质、材料特性和相关性能的某些方面。传统上，材料专家需要对这些不同信息的拼贴进行分析。然而，新出现的算法提供了一个机会，可将这些来自多种不同模式的互补测量结果融合为材料状态的整体高维描述符。我们在此提出了一个在多模态数据集中发现此类共享信息的概率框架。通过一种基于变异推理的无监督方法，我们识别出了编码跨模态相关性的语义集群，从而获得了具有物理意义的指纹，这些指纹表明了性能的不同机理机制。这种多模态性可以通过纳入基于物理的构成模型得到进一步丰富，这些模型可以促进聚类的分解。该方法的概率基础提供了不确定性量化，以评估跨模态估算的可靠性，并量化单个模态的贡献如何超过其各部分的总和。该方法针对与材料可靠性相关的三个多模态数据集进行了演示。

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