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Tailoring Mechanical Properties and Shear Band Propagation in ZrCu Metallic Glass Nanolaminates Through Chemical Heterogeneities and Interface Density 通过化学异质性和界面密度定制 ZrCu 金属玻璃纳米层压板的机械特性和剪切带传播
Pub Date : 2024-05-19 DOI: 10.1002/sstr.202400011
A. Brognara, Ankush Kashiwar, C. Jung, Xukai Zhang, Ali Ahmadian, N. Gauquelin, J. Verbeeck, Philippe Djemia, Damien Faurie, G. Dehm, H. Idrissi, J. P. Best, M. Ghidelli
The design of high‐performance structural thin films consistently seeks to achieve a delicate equilibrium by balancing outstanding mechanical properties like yield strength, ductility, and substrate adhesion, which are often mutually exclusive. Metallic glasses (MGs) with their amorphous structure have superior strength, but usually poor ductility with catastrophic failure induced by shear bands (SBs) formation. Herein, we introduce an innovative approach by synthesizing MGs characterized by large and tunable mechanical properties, pioneering a nanoengineering design based on the control of nanoscale chemical/structural heterogeneities. This is realized through a simplified model Zr24Cu76/Zr61Cu39, fully amorphous nanocomposite with controlled nanoscale periodicity (Λ, from 400 down to 5 nm), local chemistry, and glass–glass interfaces, while focusing in‐depth on the SB nucleation/propagation processes. The nanolaminates enable a fine control of the mechanical properties, and an onset of crack formation/percolation (>1.9 and 3.3%, respectively) far above the monolithic counterparts. Moreover, we show that SB propagation induces large chemical intermixing, enabling a brittle‐to‐ductile transition when Λ ≤ 50 nm, reaching remarkably large plastic deformation of 16% in compression and yield strength ≈2 GPa. Overall, the nanoengineered control of local heterogeneities leads to ultimate and tunable mechanical properties opening up a new approach for strong and ductile materials.
高性能结构薄膜的设计一直在寻求一种微妙的平衡,在屈服强度、延展性和基底附着力等出色的机械性能之间取得平衡,而这些性能往往是相互排斥的。非晶态结构的金属玻璃(MGs)具有优异的强度,但通常延展性较差,剪切带(SBs)的形成会导致灾难性的破坏。在此,我们引入了一种创新方法,通过合成具有较大和可调机械性能的 MGs,开创了一种基于纳米级化学/结构异质性控制的纳米工程设计。这是通过一种简化模型 Zr24Cu76/Zr61Cu39 全无定形纳米复合材料来实现的,该复合材料具有可控的纳米级周期性(Λ,从 400 纳米到 5 纳米)、局部化学性质和玻璃-玻璃界面,同时深入关注 SB 成核/传播过程。纳米层压板可实现对机械性能的精细控制,其裂纹形成/渗透率(分别大于 1.9% 和 3.3%)远高于单片层压板。此外,我们还发现 SB 传播会引起大量化学混杂,从而在Λ ≤ 50 nm 时实现从脆性到韧性的转变,压缩塑性变形达到显著的 16%,屈服强度≈2 GPa。总之,对局部异质性的纳米工程控制可实现最终和可调的机械性能,为开发高强度和韧性材料开辟了一条新途径。
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引用次数: 0
Improving Thermal Stability of Perovskite Solar Cells by Suppressing Ion Migration 通过抑制离子迁移提高过氧化物太阳能电池的热稳定性
Pub Date : 2024-05-16 DOI: 10.1002/sstr.202400132
Yifeng Shi, Yifan Zheng, Xun Xiao, Yan Li, Dianfu Feng, Guodong Zhang, Yang Zhang, Tao Li, Yuchuan Shao
Ion migration presents a formidable obstacle to the stability and performance of perovskite solar cells (PSCs), hindering their progress toward commercial feasibility. Herein, the degradation mechanism of PSCs caused by iodide ion migration, which leads to abnormal changes in photoluminescence transients at the buried interface of perovskite films, is investigated. In light of this problem, a novel strategy is proposed to mitigate ion migration by introducing poly(2‐vinylnaphthalene) into poly[bis(4‐phenyl)(2,4,6‐trimethylphenyl)amine] as the hole transport layer with improved ion‐blocking capability. Consequently, this layer effectively reduces defect concentration, suppresses ion migration, and modulates energy level alignment, leading to an impressive efficiency exceeding 23% for doctor‐bladed FAPbI3 PSCs. Moreover, the corresponding unencapsulated devices demonstrate remarkable durability, maintaining over 80% of their initial value after undergoing rigorous stress tests in accordance with the International Electrotechnical Commission 61215 standard for temperature, humidity, and illumination. These tests include 1000 h of thermal cycling and a long‐term operational test lasting 600 h under maximum power point tracking.
离子迁移对包晶石太阳能电池(PSCs)的稳定性和性能构成了巨大的障碍,阻碍了其商业可行性的实现。本文研究了碘离子迁移引起的 PSC 降解机制,这种迁移会导致包晶体薄膜埋藏界面的光致发光瞬态发生异常变化。针对这一问题,研究人员提出了一种新的策略,即在聚[双(4-苯基)(2,4,6-三甲基苯基)胺]中引入聚(2-乙烯基萘)作为空穴传输层,提高离子阻挡能力,从而缓解离子迁移。因此,该层能有效降低缺陷浓度、抑制离子迁移并调节能级排列,从而使刮刀式 FAPbI3 PSC 的效率超过 23%。此外,相应的未封装器件也表现出卓越的耐用性,在按照国际电工委员会 61215 标准进行严格的温度、湿度和光照应力测试后,仍能保持 80% 以上的初始值。这些测试包括 1000 小时的热循环和 600 小时的最大功率点跟踪长期运行测试。
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引用次数: 0
Low‐Temperature Epitaxy of Perovskite WO3 Thin Films under Atmospheric Conditions 大气条件下过氧化物 WO3 薄膜的低温外延
Pub Date : 2024-05-16 DOI: 10.1002/sstr.202400089
Zhuotong Sun, Ziyi Yuan, Ming Xiao, Simon M. Fairclough, Atif Jan, Giuliana Di Martino, Caterina Ducati, N. Strkalj, Judith L. MacManus‐Driscoll
As Si electronics hits fundamental performance limits, oxide integration emerges as a solution to augment the next generation of electronic and optical devices. Specifically, oxide perovskites provide diverse functionalities with a potential to create, tune, and combine emergent phenomena at interfaces. High‐level crystalline order is needed to realize these functionalities, often achieved through epitaxy. However, large‐scale implementation in consumer devices faces challenges due to the need for high‐temperature deposition in complex vacuum systems. Herein, this challenge is addressed using atmospheric pressure spatial chemical vapor deposition, a thin‐film fabrication technique that can rapidly produce uniform films at sub‐400 °C temperatures under atmospheric conditions over ≈cm2 areas. Thus, the deposition of epitaxial perovskite tungsten trioxide, WO3, thin films is demonstrated at a rate of 5 nm min−2 on single‐crystal substrates at 350 °C in open‐air conditions enabling a high‐throughput process. The resulting films exhibit crystallographic and electronic properties comparable to vacuum‐based growth above 500 °C. The high‐quality epitaxy is attributed to the energetics of the exothermic decomposition reaction of the W[CO]6 precursors combined with the stabilization of a hot zone near the substrate surface. From this work, the way can be paved for low‐temperature atmospheric‐pressure epitaxy of a wide range of other perovskite thin films.
随着硅电子器件的基本性能达到极限,氧化物集成成为增强下一代电子和光学器件的解决方案。具体来说,氧化物包晶提供了多种功能,有可能在界面上创造、调整和组合新出现的现象。要实现这些功能,需要较高的晶序,通常通过外延来实现。然而,由于需要在复杂的真空系统中进行高温沉积,消费类设备的大规模应用面临着挑战。在此,我们采用大气压空间化学气相沉积技术来应对这一挑战,这种薄膜制造技术可在大气条件下以低于 400 °C 的温度在 ≈cm2 的面积上快速生成均匀的薄膜。因此,在 350 °C 的露天条件下,以 5 nm min-2 的速度在单晶基底上沉积外延包晶三氧化钨(WO3)薄膜,实现了高通量工艺。所得薄膜的晶体学和电子特性可与 500 °C 以上的真空生长相媲美。高质量的外延归功于 W[CO]6 前驱体放热分解反应的能量学原理,以及基底表面附近热区的稳定。从这项工作出发,可以为其他各种包晶体薄膜的低温常压外延铺平道路。
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引用次数: 0
Photoinduced Dehalogenation‐Based Direct In Situ Photolithography of CsPbBr3 Quantum Dots Micropatterns for Encryption and Anti‐Counterfeiting with High Capacity 基于光诱导脱卤的原位直接光刻 CsPbBr3 量子点微图案用于高容量加密和防伪
Pub Date : 2024-05-16 DOI: 10.1002/sstr.202400078
Wanting Li, Manchun Wu, Haini Chen, Peng Zhang, Zhixiong Cai, Shunyou Cai, Feiming Li
Fluorescent lead halide perovskite quantum dots (LH PQDs) micropatterns hold great potential for photonic applications. However, current photolithography for LH PQDs micropatterning is hindered by their incompatibility with traditional photolithography methods, which involve development processes using numerous solvents and exhibit poor stability due to the ionic characteristics of LH PQDs. Herein, a direct in situ photolithography to fabricate CsPbBr3 PQDs micropatterns based on ultraviolet‐C light‐driven debromination is developed. Using this approach, fluorescent CsPbBr3 PQDs micropatterns with high theoretical information storage capacity (up to 10750205) can be achieved in a single step, without the need for tedious development processes. Furthermore, the fabricated CsPbBr3 PQDs micropatterns show high stability, remaining undamaged even after immersion in water for 6 months. The combination of excellent optical properties, development‐free process, high stability, and low cost makes the in situ photolithography strategy very promising for patterning LH PQDs toward photonic integrations.
荧光卤化铅过氧化物量子点(LH PQDs)微图案在光子应用方面具有巨大潜力。然而,目前用于 LH PQDs 微图案化的光刻技术因其与传统光刻方法不兼容而受到阻碍,传统光刻方法涉及使用大量溶剂的显影过程,并且由于 LH PQDs 的离子特性而表现出较低的稳定性。在此,我们开发了一种基于紫外 C 光驱动脱溴的直接原位光刻法来制造 CsPbBr3 PQDs 微图案。利用这种方法,无需繁琐的开发过程,只需一步就能实现具有高理论信息存储容量(高达 10750205)的荧光 CsPbBr3 PQDs 微图案。此外,制备的 CsPbBr3 PQDs 微图案显示出很高的稳定性,即使在水中浸泡 6 个月也不会损坏。出色的光学性能、免显影工艺、高稳定性和低成本的完美结合,使原位光刻技术在光子集成的 LH PQDs 图形化方面大有可为。
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引用次数: 0
Effect of Uniaxial Stack Pressure on the Performance of Nanocrystalline Electrolytes and Electrode Composites for All‐Solid‐State Fluoride‐Ion Batteries 单轴叠加压力对全固态氟离子电池用纳米晶电解质和电极复合材料性能的影响
Pub Date : 2024-05-16 DOI: 10.1002/sstr.202300570
Hong Chen, Tommi Aalto, V. Vanita, Oliver Clemens
If all‐solid‐state fluoride‐ion batteries want to compete with existing battery technologies, significant improvements in terms of cyclic stability are necessary to fully access the high specific capacities, which this battery concept can provide in theory. Herein, the development of a high‐pressure, high‐temperature battery operation stand for battery cycling under inert conditions inside a glovebox is reported. This stand is then used to investigate the effect of stack pressure on the cell performance of conversion‐based as well as intercalation‐based electrode materials for fluoride‐ion batteries. It is found that cyclic stability as well as energy efficiency is strongly increased compared to nonpressure conditions, which is assigned to sustained interparticle contact. Thus, the cell design must be considered carefully to be able to distinguish intrinsic material properties from percolation‐ and interphase‐related impacts on the cell behavior. Further, the effect of pressure on the ionic conductivity of common solid fluoride‐ion conductors is investigated.
如果全固态氟离子电池想要与现有电池技术竞争,就必须在循环稳定性方面做出重大改进,以充分获得这种电池概念理论上可以提供的高比容量。本文报告了高压高温电池操作台的开发情况,该操作台用于在手套箱内的惰性条件下进行电池循环。然后,利用该操作台研究了堆栈压力对氟离子电池转换型和插层型电极材料的电池性能的影响。研究发现,与无压条件相比,循环稳定性和能量效率都有很大提高,这归因于粒子间的持续接触。因此,必须仔细考虑电池的设计,以便能够区分材料的固有特性与渗流和相间对电池行为的影响。此外,还研究了压力对常见固体氟离子导体离子电导率的影响。
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引用次数: 0
Tuning the Optical and Photoelectrochemical Properties of Epitaxial BiVO4 by Lattice Strain 通过晶格应变调节外延 BiVO4 的光学和光电化学特性
Pub Date : 2024-05-15 DOI: 10.1002/sstr.202400097
Erwin N. Fernandez, R. van de Krol, F. Abdi
State‐of‐the‐art photoelectrodes in highly efficient photoelectrochemical (PEC) systems often comprise multilayer architectures where lattice mismatch‐imposed strain at the interfaces can perturb the material's crystalline lattice and electronic structure. Despite its inevitable presence, understanding of strain effects in semiconductor photoelectrodes is lacking, preventing rational exploitation of strain engineering to improve photoelectrode performance. In this work, we combine X‐ray structural characterization with strain tensor decomposition analysis as well as optical/photocurrent spectroscopic methods to demonstrate how volumetric lattice deformations caused by substrate‐imposed hydrostatic strain impact the optoelectronic and PEC properties of BiVO4. Utilizing single‐crystalline, epitaxial BiVO4/indium tin oxide (ITO)/yttrium‐stabilized zirconia (YSZx, x = 8% and 13% mol Y2O3) photoelectrodes as a model platform, we find that tensile hydrostatic strain that causes volumetric lattice dilation in BiVO4 results in slightly enhanced optical absorption, but it is detrimental to the internal quantum efficiencies in BiVO4. We attribute this to localization of photogenerated charge carriers, thereby leading to poor charge separation in the bulk of BiVO4 and increased recombination losses. Finally, we highlight the beneficial effects of compressive hydrostatic strain on enhancing the internal quantum efficiencies in BiVO4. Our results provide a basis for exploiting epitaxial strain engineering to optimize the performance of multilayer photoelectrodes in PEC systems.
高效光电化学(PEC)系统中最先进的光电极通常由多层结构组成,在这种结构中,晶格错配在界面处产生的应变会扰乱材料的晶格和电子结构。尽管应变不可避免地存在,但人们对半导体光电极中的应变效应还缺乏了解,因此无法合理利用应变工程来提高光电极的性能。在这项工作中,我们将 X 射线结构表征与应变张量分解分析以及光学/光电流光谱方法相结合,证明了基底施加的静水应变引起的体积晶格变形如何影响 BiVO4 的光电和 PEC 性能。利用单晶、外延 BiVO4/铟锡氧化物(ITO)/钇稳定氧化锆(YSZx,x = 8% 和 13% mol Y2O3)光电极作为模型平台,我们发现拉伸静水应变会导致 BiVO4 的体积晶格扩张,从而使光吸收略有增强,但却不利于 BiVO4 的内部量子效率。我们将其归因于光生电荷载流子的局部化,从而导致 BiVO4 体积中电荷分离不良和重组损耗增加。最后,我们强调了压缩静水应变对提高 BiVO4 内部量子效率的有利影响。我们的研究结果为利用外延应变工程优化 PEC 系统中多层光电极的性能奠定了基础。
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引用次数: 0
An Adsorptive Membrane Platform for Precision Ion Separation: Membrane Design and First‐Principles Studies 用于精确离子分离的吸附膜平台:膜设计和第一原理研究
Pub Date : 2024-05-15 DOI: 10.1002/sstr.202400067
Van T. C. Le, Quy P. Nguyen, Hien Duy Mai, Bin Wang, Ngoc T. Bui
One of the key challenges in separation science is the lack ofprecise ion separation methods and mechanistic understanding crucial for efficiently recovering critical materials from complex aqueous matrices. Herein, first‐principles electronic structure calculations and in‐situ Raman spectroscopy are studied to elucidate the factors governing ion discrimination in an adsorptive membrane specifically designed for transition metal ion separation. Density functional theory calculations and in‐situ Raman data jointly reveal the thermodynamically favorable binding preferences and detailed adsorption mechanisms for competing ions. How membrane binding preferences correlate with the electronic properties of ligands is explored, such as orbital hybridization and electron localization. The findings underscore the importance of the phenolate group in oxime ligands for achieving high selectivity among competing transition metal ions. In‐depth understanding on which specific atomistic site within the microenvironment of metal‐ligand binding pockets governs the ion discrimination behaviors of the host will build a solid foundation to guide the rational design of next‐generation materials for precision separation essential for energy technologies and environment remediation. In tandem, synthetic controllability is demonstrated to transform 3D micrometer‐scale crystals to a 2D crystalline selective layer in membranes, paving the way for more precise and sustainable advances in separation science.
分离科学面临的主要挑战之一是缺乏精确的离子分离方法以及对从复杂水基中有效回收关键材料的机理认识。本文研究了第一原理电子结构计算和原位拉曼光谱,以阐明专为分离过渡金属离子而设计的吸附膜中的离子分辨因素。密度泛函理论计算和原位拉曼数据共同揭示了竞争离子在热力学上有利的结合偏好和详细的吸附机制。研究还探讨了膜结合偏好如何与配体的电子特性相关联,如轨道杂化和电子定位。研究结果强调了肟配体中的苯酚基对于在竞争性过渡金属离子中实现高选择性的重要性。深入了解金属-配体结合袋微环境中哪个特定原子位点控制着宿主的离子鉴别行为,将为指导下一代材料的合理设计奠定坚实的基础,从而实现能源技术和环境修复所必需的精确分离。同时,研究还展示了将三维微米级晶体转化为膜中二维晶体选择层的合成可控性,为分离科学更精确、更可持续的进步铺平了道路。
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引用次数: 0
Metal Sulfide-Based Nanoarchitectures for Energetic and Environmental Applications 用于能源和环境应用的金属硫化物纳米结构
Pub Date : 2024-05-08 DOI: 10.1002/sstr.202300536
Sili Liu, Yuanli Li, Xiaoyan Zhong, Ke Yang, Xinhua Li, Wanchuan Jin, Haifeng Liu, Ruishi Xie
Despite their numerous excellent properties, metal sulfides are not particularly efficient at converting energy and purifying the environment, which limits their further applications. Fortunately, the energy conversion and environmental purification efficiencies of these materials have experienced notable advancements in recent years, accompanied by an improved understanding of their underlying mechanisms. Herein, progress in experimental researches in recent years on the engineering of single component metal sulfides by controlling morphology, construction of heterojunctions, and incorporating elements is reviewed. Methods to design and prepare metal sulfide-based composites by building binary or ternary heterojunctions of metal sulfide/semiconductor/conductor are also discussed in detail. These materials are used in energy conversion and environmental purification systems, where they act as photocatalytic materials not only to split water, reduce carbon dioxide or nitrogen, but also to degrade pollutants (organic and inorganic) in water and gas. Finally, it is concluded by summarizing the research frontiers of metal sulfide nanomaterials in energy and environmental applications, as well as proposing potential challenges and future research directions. This work may contribute to a better understanding of metal sulfide nanocomposites and provide clues for the fabrication of more efficient metal sulfide-based nanostructures for clean energy production and environmental remediation.
尽管金属硫化物具有众多优异特性,但其能量转换和环境净化效率并不高,这限制了它们的进一步应用。幸运的是,近年来,随着人们对金属硫化物内在机理认识的加深,这些材料的能量转换和环境净化效率有了显著提高。本文综述了近年来通过控制形貌、构建异质结和加入元素对单组分金属硫化物进行工程化的实验研究进展。此外,还详细讨论了通过构建金属硫化物/半导体/导体的二元或三元异质结来设计和制备基于金属硫化物的复合材料的方法。这些材料可用于能源转换和环境净化系统,作为光催化材料,它们不仅能分水、减少二氧化碳或氮气,还能降解水和气体中的污染物(有机物和无机物)。最后,总结了金属硫化物纳米材料在能源和环境应用方面的研究前沿,并提出了潜在的挑战和未来的研究方向。这项工作可能有助于更好地理解金属硫化物纳米复合材料,并为制造更高效的金属硫化物纳米结构提供线索,以用于清洁能源生产和环境修复。
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引用次数: 0
Key Roles of Initial Calcination Temperature in Accelerating the Performance in Proton Ceramic Fuel Cells via Regulating 3D Microstructure and Electronic Structure 初始煅烧温度在通过调节三维微观结构和电子结构加快质子陶瓷燃料电池性能方面的关键作用
Pub Date : 2024-05-07 DOI: 10.1002/sstr.202470020
Jingzeng Cui, Yuxuan Zhang, Ze Liu, Zhiwei Hu, Han-Ping Wang, Po-Yu Cho, Chang-Yang Kuo, Yi-Ying Chin, Chien-Te Chen, Jianqiu Zhu, Jing Zhou, Guntae Kim, Jian-Qiang Wang, Linjuan Zhang
Proton Ceramic Fuel Cells
质子陶瓷燃料电池
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引用次数: 0
Chemically Tailored Semiconductor Moiré Superlattices of Janus Heterobilayers 化学定制的半导体莫伊里超晶格简纳斯杂二层膜
Pub Date : 2024-05-07 DOI: 10.1002/sstr.202470022
Wenjin Zhang, Zheng Liu, Hiroshi Nakajo, Soma Aoki, Haonan Wang, Yanlin Wang, Yanlin Gao, Mina Maruyama, Takuto Kawakami, Yasuyuki Makino, Masahiko Kaneda, Tongmin Chen, Kohei Aso, Tomoya Ogawa, Takahiko Endo, Yusuke Nakanishi, Kenji Watanabe, Takashi Taniguchi, Yoshifumi Oshima, Yukiko Yamada-Takamura, Mikito Koshino, Susumu Okada, Kazunari Matsuda, Toshiaki Kato, Yasumitsu Miyata
Janus Heterobilayers
雅努斯异形
{"title":"Chemically Tailored Semiconductor Moiré Superlattices of Janus Heterobilayers","authors":"Wenjin Zhang, Zheng Liu, Hiroshi Nakajo, Soma Aoki, Haonan Wang, Yanlin Wang, Yanlin Gao, Mina Maruyama, Takuto Kawakami, Yasuyuki Makino, Masahiko Kaneda, Tongmin Chen, Kohei Aso, Tomoya Ogawa, Takahiko Endo, Yusuke Nakanishi, Kenji Watanabe, Takashi Taniguchi, Yoshifumi Oshima, Yukiko Yamada-Takamura, Mikito Koshino, Susumu Okada, Kazunari Matsuda, Toshiaki Kato, Yasumitsu Miyata","doi":"10.1002/sstr.202470022","DOIUrl":"https://doi.org/10.1002/sstr.202470022","url":null,"abstract":"<b>Janus Heterobilayers</b>","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140930085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Small Structures
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