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Multifold Fermions Boosted Hydrogen Evolution Reaction Catalysis in Cubic Palladium Bronze LaPd3S4 多倍费米子促进立方钯青铜 LaPd3S4 中的氢气进化反应催化作用
Pub Date : 2024-09-09 DOI: 10.1002/sstr.202470041
Yang Li, Jialin Gong, Xiaotian Wang
Topological Catalysis
拓扑催化
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引用次数: 0
Inkjet-Printed Flexible and Transparent Ti3C2Tx/TiO2 Composite Films: A Strategy for Photoelectrically Controllable Photocatalytic Degradation 喷墨打印的柔性透明 Ti3C2Tx/TiO2 复合薄膜:光电可控光催化降解策略
Pub Date : 2024-09-09 DOI: 10.1002/sstr.202400214
Ziying Ji, Yiran Wu, Lu Liu, Wei Zheng, Meng Wu, Yuexia Li, Zhengming Sun, Guobing Ying
The 2D Ti3C2Tx MXene has a large specific surface area, abundant functional groups, and low work function, which has potential in the field of photocatalytic materials. However, the manufacturing of controllable films with high photocatalytic properties and desirable transmittance is a challenging task. Herein, low-cost, large-scale, and rapid preparation of Ti3C2Tx/TiO2 flexible composite films have been successfully prepared by inkjet printing technology, which can be applied in complex and special environments, as well as in photoelectrically controllable places for photocatalytic performance. With the increase of the anatase TiO2, the transmittance of Ti3C2Tx/TiO2 films increases from 55.37% to 73.27% at 780 nm, corresponding to the square resistance of 1.112–206.496 kΩ sq−1 and the figure of merit of 0.48–0.005. When the amount of anatase TiO2 is 15%, the film has the best photocatalytic effect on methylene blue (MB) dye, reaching 68.94%. After five cycles of testing, the degradation efficiency of MB dye decreases by only 5.68%, showing that the film has good cycling stability. This work provides a new research direction for photoelectrically controllable photocatalytic degradation in complex and special environments.
二维 Ti3C2Tx MXene 具有较大的比表面积、丰富的官能团和较低的功函数,在光催化材料领域具有潜力。然而,制造具有高光催化性能和理想透光率的可控薄膜是一项具有挑战性的任务。本文利用喷墨打印技术成功制备了低成本、大规模、快速制备的Ti3C2Tx/TiO2柔性复合薄膜,可应用于复杂、特殊环境以及光电可控场所的光催化性能。随着锐钛矿二氧化钛含量的增加,Ti3C2Tx/TiO2 薄膜在 780 纳米波长下的透过率从 55.37% 增加到 73.27%,对应的平方电阻为 1.112-206.496 kΩ sq-1,优点系数为 0.48-0.005。当锐钛型二氧化钛的用量为 15%时,薄膜对亚甲基蓝(MB)染料的光催化效果最好,达到 68.94%。经过五个循环测试后,MB 染料的降解效率仅下降 5.68%,表明薄膜具有良好的循环稳定性。这项工作为复杂和特殊环境下的光电可控光催化降解提供了新的研究方向。
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引用次数: 0
Covalently Linked Pigment@TiO2 Hybrid Materials by One-Pot Solvothermal Synthesis 通过一锅溶热合成实现共价连接的颜料@TiO2 混合材料
Pub Date : 2024-09-09 DOI: 10.1002/sstr.202470043
Frank Sailer, Hipassia M. Moura, Taniya Purkait, Lars Vogelsang, Markus Sauer, Annette Foelske, Rainer F. Winter, Alexandre Ponrouch, Miriam M. Unterlass
Hybrid Materials
混合材料
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引用次数: 0
Small-Molecule Polycyclic Aromatic Hydrocarbons as Exceptional Long-Cycle-Life Li-Ion Battery Anode Materials 作为特殊长循环寿命锂离子电池阳极材料的小分子多环芳烃
Pub Date : 2024-09-09 DOI: 10.1002/sstr.202400273
Avi Arya, Sih-Ling Hsu, Chi-You Liu, Meng-Yuan Chang, Jeng-Kuei Chang, Elise Yu-Tzu Li, Yu-Sheng Su
The growing demand for cost-effective and sustainable energy-storage solutions has spurred interest in novel anode materials for lithium-ion batteries (LIBs). In this study, the potential of small-molecule polycyclic aromatic hydrocarbons (SMPAHs) as promising candidates for LIB anodes is explored. Through a comprehensive experimental approach involving electrode fabrication, material characterization, and electrochemical testing, the electrochemical performance of SMPAHs, including naphthalene, biphenyl, 9,9-dimethylfluorene, phenanthrene, p-terphenyl, and pyrene (Py), is thoroughly investigated. In the results, the impressive cycle stability, high specific capacity, and excellent rate capability of the SMPAH electrode are revealed. Additionally, a direct contact prelithiation strategy is implemented to enhance the initial Coulombic efficiency (ICE) of SMPAH anodes, yielding significant improvements in the ICE and cycle stability. Computational simulations provide valuable insights into the electrochemical behavior and lithium-storage mechanisms of SMPAHs, confirming their potential as effective anode materials. The simulations reveal favorable lithium adsorption sites, the predominant storage mechanisms, and the dissolution mechanism of Py through computational calculations. Overall, in this study, the promise of SMPAHs is highlighted as sustainable anode materials for LIBs, advancing energy-storage technologies toward a greener future.
对具有成本效益和可持续能源存储解决方案的需求日益增长,激发了人们对新型锂离子电池(LIB)负极材料的兴趣。本研究探讨了小分子多环芳烃(SMPAHs)作为锂离子电池阳极候选材料的潜力。通过涉及电极制造、材料表征和电化学测试的综合实验方法,深入研究了 SMPAHs(包括萘、联苯、9,9-二甲基芴、菲、对三联苯和芘)的电化学性能。研究结果表明,SMPAH 电极具有令人印象深刻的循环稳定性、高比容量和出色的速率能力。此外,为了提高 SMPAH 阳极的初始库仑效率 (ICE),还采用了直接接触预硫化策略,从而显著提高了 ICE 和循环稳定性。计算模拟为了解 SMPAH 的电化学行为和锂存储机制提供了宝贵的见解,证实了它们作为有效负极材料的潜力。模拟计算揭示了有利的锂吸附位点、主要的储存机制以及 Py 的溶解机制。总之,本研究强调了 SMPAHs 作为可持续锂离子电池负极材料的前景,从而推动储能技术走向更加绿色的未来。
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引用次数: 0
Spatially Selective Ultraprecision Polishing and Cleaning by Collective Behavior of Micro Spinbots 利用微旋机器人的集体行为进行空间选择性超精密抛光和清洁
Pub Date : 2024-09-09 DOI: 10.1002/sstr.202400245
Hyeongmin Je, Sukyoung Won, Jeong Jae Wie, Sanha Kim
Untethered magnetic actuation is an attractive technique for controlling a batch of micrometer-sized soft robots. Recent advancements have enabled each robot to follow its path independently using a single magnetic device. However, applications of magnetic soft microrobots are mostly biased toward the biomedical field. In this study, thermoplastic polyurethane–Fe3O4 nanocomposite soft spinning microrobots, that is, spinbots that actuate on a tabletop magnetic stirrer, were utilized as innovative precision manufacturing tools for spatially selective precision polishing and cleaning. The pivot motion of the revolving spinbots, which involves repetitive sweeping during rotation cycles, is explored. This sweeping action physically removes nanometer-sized surface contaminants from the workpiece, achieving a cleaning efficiency of 99.6%. Multiple spinbots, up to 42 in total, simultaneously operated along their own orbital pathways on three vertically stacked wafers, thereby demonstrating an unprecedented cleaning method. In addition, the spinbots precisely removed materials from the workpiece using a three-body abrasion mechanism. Furthermore, the spinbots contributed to precise material removal, resulting in remarkable surface polishing (Ra ≈ 1.8 nm). This novel polishing system, which uses the collective behavior of multiple spinbots on a tabletop magnetic stirrer, is 1000-fold lighter than current state-of-the-art equipment aimed at achieving similar levels of fine finishing.
对于控制一批微米大小的软体机器人来说,无系磁力驱动是一项极具吸引力的技术。最近的进步使每个机器人都能使用单个磁性装置独立地沿着自己的路径前进。然而,磁性软微型机器人的应用大多偏向于生物医学领域。在这项研究中,热塑性聚氨酯-Fe3O4 纳米复合软旋转微机器人(即在桌面磁力搅拌器上驱动的旋转机器人)被用作创新的精密制造工具,用于空间选择性精密抛光和清洁。研究探讨了旋转旋转机器人的枢轴运动,其中包括在旋转周期内的重复清扫。这种清扫动作可物理去除工件上纳米级的表面污染物,清洁效率高达 99.6%。在三个垂直堆叠的晶片上,多个旋转机器人(总共多达 42 个)沿着各自的轨道路径同时运行,从而展示了一种前所未有的清洁方法。此外,自旋机器人还利用三体磨损机制精确地清除了工件上的材料。此外,自旋机器人还有助于精确去除材料,从而实现了出色的表面抛光(Ra ≈ 1.8 nm)。这种新颖的抛光系统利用台式磁力搅拌器上多个自旋机器人的集体行为,比目前旨在实现类似精细抛光水平的最先进设备轻 1000 倍。
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引用次数: 0
Single Site W(0) versus Re(I)-Dipyridophenazine- Based Conjugated Porous Polymer for CO2 Photoreduction 用于二氧化碳光还原的单位点 W(0) 与 Re(I)- 二哒嗪基共轭多孔聚合物
Pub Date : 2024-09-09 DOI: 10.1002/sstr.202400185
Ángela Matarín, Félix Sánchez, Laura Collado, Mariam Barawi, Victor A. de la Peña O'Shea, Avelina Arnanz, Marta Liras, Marta Iglesias
Herein, the synthesis and characterization of two robust tungsten and rhenium carbonyl complexes integrated into an organic polymer (CPP-Re, CPP-W) are reported. These polymers are obtained by a Suzuki coupling reaction between the corresponding dibromo metal-carbonyl substituted dipyrido[3,2-a:2′,3′-c]phenazine complex and 1,3,5-triphenylbenzene-4′,4″,4″,4‴-triboronic acid and integrated catalytic active sites and photosensitizer since they have not only nitrogen sites to coordinate metal active centers as rhenium or tungsten but photoactive units with good charge-separating ability which can significantly improve the CO2 photoreduction reaction (CO2PRR). These polymers show similar activity in solid–gas CO2PRR in absence of sacrificial agents to produce syn gas (CO + H2) but CPP-W selectivity to products change regarding CPP-Re being able to produce also large amount of more demanding electron products such as methane and ethane. Moreover, the single-site Re- or W-CPP catalysts could prevent the dimerization of complexes that produces its deactivation. This work shows the potential of CPPs as matrices to support single active centers for heterogeneous catalysis.
本文报告了集成到有机聚合物(CPP-Re、CPP-W)中的两种坚固的钨和铼羰基复合物的合成和表征。这些聚合物是通过相应的二溴金属羰基取代二吡啶并[3,2-a:2′,3′-c]吩嗪络合物和 1,3,5-三苯基苯-4′,4″,4″,4‴-三硼酸之间的铃木偶联反应得到的,并集成了催化活性位点和光敏剂,因为它们不仅具有氮位点来配位金属活性中心(如铼或钨),还具有具有良好电荷分离能力的光活性单元,可显著改善二氧化碳光还原反应(CO2PRR)。在没有牺牲剂的情况下,这些聚合物在固体气体 CO2PRR 中显示出类似的活性,可产生合成气体(CO + H2),但 CPP-W 对产物的选择性发生了变化,CPP-Re 还能产生大量对电子要求更高的产物,如甲烷和乙烷。此外,单位点 Re- 或 W-CPP 催化剂可以防止复合物二聚化而导致失活。这项工作显示了 CPP 作为基质支持单活性中心进行异相催化的潜力。
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引用次数: 0
Unveiling Inequality of Atoms in Ultrasmall Pt Clusters: Oxygen Adsorption Limited to the Uppermost Atomic Layer 揭示超小铂团簇中原子的不平等性:氧吸附仅限于原子最上层
Pub Date : 2024-09-09 DOI: 10.1002/sstr.202400250
Federico Loi, Luca Bignardi, Deborah Perco, Andrea Berti, Paolo Lacovig, Silvano Lizzit, Aras Kartouzian, Ulrich Heiz, Dario Alfè, Alessandro Baraldi
The concept of preferential atomic and molecular adsorption site is of primary relevance in heterogeneous catalysis. In the case of ultrasmall size-selected clusters, distinguishing the role played by each atom in a reaction is extremely challenging due to their reduced size and peculiar structures. Herein, it is revealed how the inequivalent atoms composing graphene-supported Pt12 and Pt13 clusters behave differently in the photoinduced dissociation of O2, with only those in the uppermost layer of the clusters being involved in the reaction. In this process, the epitaxial graphene support plays a fundamental active role: its corrugation and pinning induced by the presence of the clusters are crucial for defining the preferential adsorption site on the Pt atomic agglomerates, facilitating the lateral diffusion of physisorbed oxygen at a distance that induces its selective adsorption in the topmost layer of the clusters, and inducing an inhomogeneous charge distribution within the clusters which directly affects the O2 adsorption. The inhomogeneous oxidation of the clusters is resolved by means of synchrotron-based X-ray photoelectron spectroscopy and supported by ab initio density functional theory calculations. The possibility to identify the active sites on Pt clusters induced by cluster–support interactions has the potential to enhance the experimentally supported design of nanocatalysts.
原子和分子优先吸附位点的概念在异相催化中具有重要意义。对于超小尺寸的选择性团簇,由于其尺寸减小、结构特殊,区分每个原子在反应中的作用极具挑战性。本文揭示了组成石墨烯支持的 Pt12 和 Pt13 团簇的不等价原子在光诱导解离 O2 的过程中的不同表现,其中只有团簇最上层的原子参与了反应。在这一过程中,外延石墨烯支撑起着根本性的积极作用:簇群的存在所诱导的石墨烯波纹和针刺对于确定铂原子团聚体上的优先吸附位点至关重要,促进了物理吸附氧的横向扩散距离,从而诱导其选择性地吸附在簇群的最上层,并诱导簇群内部的不均匀电荷分布,这直接影响了对 O2 的吸附。通过同步辐射 X 射线光电子能谱分析和非初始密度泛函理论计算,解决了集群的非均相氧化问题。确定铂团簇上由团簇-支撑相互作用诱导的活性位点的可能性有望提高纳米催化剂设计的实验支持水平。
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引用次数: 0
Deep-Learning-Assisted Affinity Classification for Humoral Immunoprotein Complexes 深度学习辅助的体液免疫蛋白复合物亲和力分类
Pub Date : 2024-09-09 DOI: 10.1002/sstr.202400204
Bahar Dadfar, Safoura Vaez, Cristian Haret, Meike Koenig, Tahereh Mohammadi Hafshejani, Matthias Franzreb, Joerg Lahann
Immunoglobulins are important building blocks in biology and biotechnology. With the emergence of comprehensive deep-learning approaches, there are enormous opportunities for fast and accurate methods of classification of protein–protein interactions to arise. Herein, widely accessible image classification algorithms for species-specific typification of a range of different immunoglobulin G (IgG) complexes are repurposed. Droplets of various immunoglobulins mixed with a B-cell superantigen (SAg) (recombinant staphylococcal Protein A) are deposited onto hydrophobic polymer substrates and the resulting protein stains are imaged using polarized light microscopy. A comprehensive study based on 23 745 images finds that the pretrained convolutional neural network (CNN) InceptionV3 not only successfully categorizes IgGs from four different species but also predicts their binding affinity to Protein A: averaged over 36 binding pairs, the following are observed: 1) an overall accuracy of 81.4%, 2) the highest prediction accuracy for human IgG, the antibody with the highest binding affinity for Protein A, and 3) that the classification accuracy regarding the various IgG/Protein A ratios generally correlates with the binding strength of the protein–protein–complex as determined via circular dichroism spectroscopy. In addition, the CNN pretrained with IgG/Protein A stain images has been challenged with a new set of images using a different superantigen (SAg, Protein G). Despite the use of the unknown SAg, the CNN correctly classifies the images of human IgG and Protein G as indicated by a 94% accuracy over the various molar binding ratios. These findings are noteworthy because they demonstrate that appropriately pretrained CNNs can be used for the prediction of protein–protein interactions beyond the scope of the original training set. Aided by deep-learning methods, simple stains of mixed protein solutions may serve as accurate predictors of the strength of protein–protein interactions with relevance to protein engineering, self-aggregation, or protein stability in complex media.
免疫球蛋白是生物学和生物技术的重要组成部分。随着综合深度学习方法的出现,出现了快速、准确的蛋白质-蛋白质相互作用分类方法的巨大机遇。在此,我们将广泛使用的图像分类算法重新用于对一系列不同的免疫球蛋白 G(IgG)复合物进行物种特异性分型。将各种免疫球蛋白与 B 细胞超抗原(SAg)(重组葡萄球菌蛋白 A)混合后的液滴沉积在疏水性聚合物基底上,并使用偏振光显微镜对所产生的蛋白染色进行成像。一项基于 23 745 张图像的综合研究发现,预训练卷积神经网络(CNN)InceptionV3 不仅能成功地对来自四个不同物种的 IgG 进行分类,还能预测它们与蛋白 A 的结合亲和力:对 36 对结合对进行平均,观察到以下结果:1) 整体准确率为 81.4%;2) 人类 IgG 的预测准确率最高,它是与蛋白 A 结合亲和力最高的抗体;3) 不同 IgG/Protein A 比率的分类准确率通常与通过圆二色光谱测定的蛋白质-蛋白质-复合物的结合强度相关。此外,使用不同超抗原(SAg,蛋白质 G)的一组新图像对使用 IgG/Protein A 染色图像预训练的 CNN 进行了挑战。尽管使用了未知的 SAg,但 CNN 仍能正确地对人类 IgG 和蛋白质 G 的图像进行分类,在各种摩尔结合率下的准确率高达 94%。这些发现值得注意,因为它们证明了经过适当预训练的 CNN 可用于预测超出原始训练集范围的蛋白质-蛋白质相互作用。在深度学习方法的帮助下,混合蛋白质溶液的简单染色可以准确预测蛋白质-蛋白质相互作用的强度,这与蛋白质工程、自聚集或蛋白质在复杂介质中的稳定性息息相关。
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引用次数: 0
Gas-Shearing Microfluidic Fabrication of Polydiacetylene–Alginate Colorimetric Sensor Beads 用气剪微流控技术制造聚二乙炔-海藻酸盐比色传感器微珠
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400340
Narges Ahmadi, Dong Yun Kim, Seung Soo Shin, Sneha Daradmare, Jong-Man Kim, Bum Jun Park
Polydiacetylenes (PDA) are highly regarded for their unique colorimetric and fluorescent responses, making them ideal for sensor development. Despite their potential, conventional methods for fabricating biocompatible PDA-encapsulated hydrogel sensor beads often fail to offer precise control over bead size and morphology. This study introduces a coflow gas-shearing microfluidic system that effectively overcomes these limitations, enabling the controlled production of polydiacetylene/alginate (PDA/Alg) and polydiacetylene/polydimethylsiloxane/alginate (PDA/PDMS/Alg) microbeads. Through systematic variation of gas pressure, liquid flow rates, and nozzle sizes, the mechanisms of droplet breakup and generation are explored. This process is validated through numerical modeling based on the Weber number, which enhances our understanding of droplet size distribution and flow regimes. The solvatochromic properties of PDA/Alg microbeads are assessed, highlighting their potential as polar solvent sensors and discussing the solvatochromic mechanism in terms of intermolecular interactions and the dissolution of unpolymerized monomers. Additionally, PDA/PDMS/Alg microbeads exhibit a semireversible thermochromic response under repeated cycles of heating, cooling, and UV exposure. This response is attributed to the formation of new PDA domains inside the PDMS phase upon UV exposure onto the red-phase microbeads. Overall, this study successfully demonstrates a straightforward and effective microfluidic approach for producing well-defined stimulus-responsive PDA–hydrogel microbeads.
聚二甲苯(PDA)因其独特的比色和荧光反应而备受推崇,是开发传感器的理想材料。尽管具有潜力,但制造生物相容性 PDA 包裹水凝胶传感器珠的传统方法往往无法精确控制珠子的大小和形态。本研究介绍了一种共流气体剪切微流体系统,它能有效克服这些限制,实现聚二乙烯/精氨酸(PDA/Alg)和聚二乙烯/聚二甲基硅氧烷/精氨酸(PDA/PDMS/Alg)微珠的可控生产。通过系统地改变气体压力、液体流速和喷嘴尺寸,探索了液滴破裂和生成的机理。这一过程通过基于韦伯数的数值建模得到了验证,从而加深了我们对液滴大小分布和流动机制的理解。评估了 PDA/Alg 微珠的溶变色特性,突出了其作为极性溶剂传感器的潜力,并从分子间相互作用和未聚合单体溶解的角度讨论了溶变色机制。此外,PDA/PDMS/Alg 微珠在加热、冷却和紫外线照射的反复循环下表现出半可逆的热致变色反应。这种反应是由于红相微珠经紫外线照射后,在 PDMS 相内形成了新的 PDA 域。总之,这项研究成功地展示了一种直接有效的微流控方法,用于生产定义明确的刺激响应型 PDA 水凝胶微珠。
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引用次数: 0
Negative Charge Carbon Dots Manufacturing Electrostatic Shielding Layer for Stable Zinc Anode 负电荷碳点为稳定的锌阳极制造静电屏蔽层
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400343
Kai Wang, Jinqiang Gao, Huaxin Liu, Weishun Jian, Jiangnan Huang, XinYu Hu, Siyuan Lai, Yafei Li, Guoqiang Zou, Hongshuai Hou, Wentao Deng, Xiaobo Ji
Alkaline zinc-based batteries (AZBs) can yield higher operating voltages due to a more negative electrode potential of zinc metal in alkaline electrolytes compared with neutral electrolytes, delivering high energy density in practical manufacturing applications. However, AZBs also exhibit more pronounced problems due to severe corrosion of the zinc anode by the strongly alkaline electrolyte environment. Combined with the reaction mechanism of alkaline zinc batteries, negatively charged carbon dots are innovatively used to construct a barrier with both physical and chemical effects. Zinc anode exposure to electrolyte is reduced by superior barrier, which assures transmission of zinc ions rather than zincate ions through electrostatic force balance, thus improving the distribution of the electric field for zinc ion deposition as well as avoiding accumulation of zincate ions at the interface. The number of harmful dendrite formation was found to be significantly suppressed by in situ optical microscopy. When coupled with silver oxide cathode for testing, the assembled silver-zinc battery results in a significant enhancement in its cyclic life. It is believed that this study will propel the development of zinc anode in alkaline batteries and provide new insights for their application.
与中性电解质相比,碱性电解质中锌金属的电极电位更负,因此碱性锌基电池(AZB)可以产生更高的工作电压,从而在实际生产应用中提供高能量密度。然而,AZB 也会因强碱性电解质环境对锌阳极的严重腐蚀而产生更明显的问题。结合碱性锌电池的反应机理,带负电荷的碳点被创新性地用于构建具有物理和化学效应的阻挡层。锌阳极暴露在电解液中的机会因卓越的阻挡层而减少,阻挡层通过静电力平衡确保了锌离子而非锌酸根离子的传输,从而改善了锌离子沉积的电场分布,并避免了锌酸根离子在界面上的积累。原位光学显微镜发现,有害枝晶的形成数量明显减少。在与氧化银阴极一起进行测试时,组装后的银锌电池的循环寿命显著提高。相信这项研究将推动碱性电池中锌阳极的发展,并为其应用提供新的见解。
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引用次数: 0
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Small Structures
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