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In Situ Bipolar Doping via Mechanically Controlled Dipole Under Water 通过水下机械控制偶极实现原位双极掺杂
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-05-02 DOI: 10.1002/admi.202301092
Sanghwan Choi, Gunhoo Woo, Taesung Kim

Polycrystalline silicon (poly-Si) is essential in integrated circuits and microelectromechanical systems. In addition, poly-Si is gaining attention for next-generation display research with high thermal conductivity, stability, and versatile applications. Conventional fabrication methods for doping patterns involve complex lithography and chemical usage, which have raised environmental concerns. The study of novel methods is necessary for environmental friendliness and a significant simplification of the manufacturing processes. This study introduces a novel bipolar work function control technology utilizing deionized water (DI-W) and nanonewton-scale mechanical force using an atomic force microscope. The method is implemented with a mechanically induced SiOx layer on poly-Si in DI-W. The induced Si─OH and Si─O bonds decreases the work function, whereas a thicker SiOx layer with a high oxidation state increases the work function. Based on the magnitude of the applied force (26.73–75.24 nN) and additional DI-W immersion, the induced bond and thickness of the SiOx layer are controlled. Therefore, bipolar work function control is achieved in the range of −0.25–+0.103 eV. In addition, the electrical characteristics of the fabricated p- and n-type poly-Si diodes are investigated. This method is eco-friendly and enables bipolar doping patterns in a single process with high efficiency.

多晶硅(Poly-Si)在集成电路和微机电系统中至关重要。此外,多晶硅还具有高热导率、高稳定性和应用广泛等特点,在下一代显示器研究中正受到越来越多的关注。掺杂图案的传统制造方法涉及复杂的光刻技术和化学使用,引起了环境问题。为了实现环境友好和制造工艺的显著简化,有必要研究新型方法。本研究介绍了一种利用去离子水(DI-W)和原子力显微镜的纳牛顿级机械力的新型双极工作函数控制技术。该方法是在去离子水中的多晶硅上使用机械诱导氧化硅层来实现的。诱导的 Si─OH 和 Si─O 键降低了功函数,而具有高氧化态的较厚氧化硅层则增加了功函数。根据施加力的大小(26.73-75.24 nN)和额外的 DI-W 浸入,可以控制诱导键和氧化硅层的厚度。因此,在 -0.25-+0.103 eV 范围内实现了双极功函数控制。此外,还研究了所制造的 p 型和 n 型多晶硅二极管的电气特性。这种方法对环境友好,可在单一工艺中高效实现双极掺杂模式。
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引用次数: 0
Stability of Immobilized Chemosensor‐Filled Vesicles on Anti‐Fouling Polymer Brush Surfaces 防污聚合物刷表面固定化化学传感器填充囊泡的稳定性
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-05-02 DOI: 10.1002/admi.202400200
Wenwu Yang, Jiangxiong Xiao, Bingquan Yang, George Mathew, Andreas H. Schäfer, Michael Hirtz
The characterization of phospholipid membrane permeability for small molecules is crucial for many applications in drug discovery and biomedical research in general. Here, chemosensor‐laden vesicles offer an attractive platform for permeability assays. In this work, the stability of immobilized chemosensor‐filled vesicles is explored on anti‐fouling polymer brush surfaces for potential use in monitoring small molecule membrane permeability. The study focuses on the development of a method for immobilizing sensor‐loaded vesicles into arbitrary patterns on surfaces and characterizing their stability under changing temperatures and compositions. As substrate to enable intact, long‐term stable vesicle immobilization reactive polymer brushes with anti‐fouling properties are used. Utilizing microchannel cantilever spotting, biotin moieties are introduced on the polymer brush surface, enabling stable tethering of vesicles through streptavidin‐biotin interactions. The immobilized vesicles are monitored through fluorescence microscopy for their response to analytes under changing environmental parameters and vesicle composition. A higher stability of immobilized vesicles compared to free‐floating ones is observed, with permeability only at elevated temperatures. By tuning vesicle compositions, permeability at lower temperatures can be raised again. Overall, the study provides insights into a novel approach for vesicle immobilization, showcasing the potential of surface‐bound vesicles for applications in microfluidic systems and as biosensors in various assays.
磷脂膜对小分子渗透性的表征对于药物发现和生物医学研究的许多应用至关重要。在此,化学传感器填充囊泡为渗透性检测提供了一个极具吸引力的平台。在这项研究中,我们探讨了在防污聚合物刷表面上固定化学传感器填充囊泡的稳定性,以便用于监测小分子膜渗透性。研究的重点是开发一种方法,将装有传感器的囊泡固定在表面上的任意图案中,并表征其在温度和成分变化时的稳定性。为了实现完整、长期稳定的囊泡固定,使用了具有防污特性的活性聚合物刷作为基底。利用微通道悬臂点焊技术,在聚合物刷表面引入生物素分子,通过链霉亲和素-生物素的相互作用实现囊泡的稳定系留。在环境参数和囊泡组成不断变化的情况下,通过荧光显微镜监测固定化囊泡对分析物的反应。与自由浮动的囊泡相比,固定化囊泡的稳定性更高,只有在温度升高时才具有渗透性。通过调整囊泡成分,可以再次提高低温下的渗透性。总之,这项研究为囊泡固定化的新方法提供了见解,展示了表面结合囊泡在微流体系统中的应用潜力,以及在各种检测中作为生物传感器的潜力。
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引用次数: 0
Quaternary Ammonium Compounds and Their Composites in Antimicrobial Applications 抗菌应用中的季铵盐化合物及其复合材料
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-05-01 DOI: 10.1002/admi.202300946
Yining Yao, Zilin Ye, Yue Zhang, Yue Wang, Chengzhong Yu

Quaternary ammonium compounds (QACs) are well-known for their antimicrobial properties, but their widespread use is limited due to suboptimal antimicrobial efficiency and safety concerns. Recent progress in materials science has paved the way for the development of QAC-based composites (QACCs). QACCs with diverse compositions have shown enhanced antimicrobial effectiveness and biosafety for various applications, such as food packaging, capacitive deionization, and household antimicrobials. This review provides a comprehensive summary of the synthesis approaches and different types of QACCs. Moreover, this review examines their antimicrobial applications, taking the underlying structure-activity relationship into consideration. In addition, this perspectives are presented on the remaining challenges and future research directions for the further development of QACCs. It is expected that this review will provide a valuable reference for the design of next generation QACC-based antimicrobial agents.

季铵盐化合物(QAC)以其抗菌特性而闻名,但由于抗菌效率不理想和安全问题,其广泛应用受到限制。材料科学的最新进展为开发基于 QAC 的复合材料(QACCs)铺平了道路。不同成分的 QACC 在食品包装、电容式去离子和家用抗菌剂等各种应用中显示出更强的抗菌效果和生物安全性。本综述全面总结了 QACC 的合成方法和不同类型。此外,本综述还考虑到其基本的结构-活性关系,对其抗菌应用进行了研究。此外,本综述还对进一步开发 QACCs 所面临的挑战和未来的研究方向进行了展望。希望本综述能为设计基于 QACC 的下一代抗菌剂提供有价值的参考。
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引用次数: 0
Ribogreen Fluorescent Assay Kinetics to Measure Ribonucleic Acid Loading into Lipid Nanoparticle Carriers 测定核糖核酸载入脂质纳米颗粒载体的核糖核酸荧光测定动力学
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-04-30 DOI: 10.1002/admi.202301083
Navid Bizmark, Satya Nayagam, Bumjun Kim, David F. Amelemah, Dawei Zhang, Sujit S. Datta, Rodney D. Priestley, Tom Colace, Jane Wang, Robert K. Prud'homme

New generations of vaccines have been developed by encapsulating messenger ribonucleic acid (mRNA) in lipid nanoparticle (LNP) carriers. In addition to the physicochemical properties of LNPs, the encapsulation efficiency (EE) of mRNA in LNPs is a key factor to screen vaccine assembly assays. Fluorescent dyes with amplified signals upon binding with mRNA are at the core of developing assays to quantify EE. However, disregarding the temporal effects during the assay impacts the accuracy of the assay. Here, the kinetics of temporal decay in fluorescence intensity of dye-RNA complex—in Ribogreen assay—are reported and shown how this dynamic process can be impeded in the presence of a nonionic surfactant. Further, the impact of this dynamic process on the calculated EE is studied. The corrections needed to accurately assay dynamic mRNA loading processes are presented.

将信使核糖核酸(mRNA)封装在脂质纳米粒子(LNP)载体中开发出了新一代疫苗。除了 LNPs 的物理化学特性外,mRNA 在 LNPs 中的封装效率 (EE) 也是筛选疫苗组装试验的关键因素。与 mRNA 结合后信号放大的荧光染料是开发量化 EE 的检测方法的核心。然而,在检测过程中忽略时间效应会影响检测的准确性。本文报告了 Ribogreen 检测法中染料-RNA 复合物荧光强度的时间衰减动力学,并展示了非离子表面活性剂存在时如何阻碍这一动态过程。此外,还研究了这一动态过程对计算 EE 的影响。报告还介绍了准确测定动态 mRNA 负载过程所需的校正。
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引用次数: 0
Probing the Interfacial Molecular Structure of a Co-Prussian Blue In Situ 原位探测共普鲁士蓝的界面分子结构
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-04-29 DOI: 10.1002/admi.202400009
Anupam Bera, Ratnadip De, Heiner Schmidt, Desirée Leistenschneider, Turkan Gamze Ulusoy Ghobadi, Martin Oschatz, Ferdi Karadaş, Benjamin Dietzek-Ivanšić
Molecular-level insight into the interfacial composition of electrodes at the solid-electrolyte and the solid-electrode interface is essential to understanding the charge transfer processes, which are vital for electrochemical (EC) and photoelectrochemical (PEC) applications. However, spectroscopic access to both interfaces, particularly upon application of an external bias, remains a challenge. Here, in situ surface sensitive vibrational sum-frequency generation (VSFG) spectroscopy is used for the first time to directly access the interfacial structure of a cobalt-containing Prussian blue analog (Co-PBA) in contact with the electrolyte and TiO2/Au surface. Structural and compositional changes of the Prussian blue layer during electrochemical oxidation are studied by monitoring the stretching vibration of the CN group. At open circuit potential, VSFG reveals a non-homogeneous distribution of oxidation states of metal sites: FeIII–CN–CoII and FeII–CN–CoIII coordination motifs are dominantly observed at the Co-PBA|TiO2 interface, while it is only the FeII–CN–CoII unit at the electrolyte interface. Upon increasing the potential applied to the electrode, the partial oxidation of FeII–CN–CoII to FeIII–CN–CoII is observed followed by its transformation to FeII–CN–CoIII via charge transfer and, finally, the formation of FeIII–CN–CoIII species at the interface with TiO2 and the electrolyte.
从分子水平深入了解电极在固体-电解质和固体-电极界面上的界面成分,对于理解电荷转移过程至关重要,而电荷转移过程对于电化学(EC)和光电化学(PEC)应用也至关重要。然而,对这两个界面进行光谱分析,尤其是在施加外部偏压时,仍然是一项挑战。本文首次采用原位表面敏感振动总频发生(VSFG)光谱技术,直接获取与电解质和 TiO2/Au 表面接触的含钴普鲁士蓝类似物(Co-PBA)的界面结构。通过监测 CN 基团的伸缩振动,研究了电化学氧化过程中普鲁士蓝层的结构和组成变化。在开路电位下,VSFG 揭示了金属位点氧化态的非均相分布:在 Co-PBA|TiO2 界面主要观察到 FeIII-CN-CoII 和 FeII-CN-CoIII 配位基团,而在电解质界面仅观察到 FeII-CN-CoII 单元。当电极上的电位升高时,FeII-CN-CoII 部分氧化为 FeIII-CN-CoII,然后通过电荷转移转变为 FeII-CN-CoIII,最后在 TiO2 和电解质界面上形成 FeIII-CN-CoIII 物种。
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引用次数: 0
Long‐Term Immersion Study for Durability of Interconnected Micropatterned Surfaces with Sustained Water Repellency 互联微图案表面持续防水耐久性的长期浸泡研究
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-04-28 DOI: 10.1002/admi.202400144
Seo Rim Park, Seungmin Oh, Woo Young Kim, Do Hyeog Kim, Sang Hoon Lee, Seungwoo Shin, Su Hyun Choi, Sin Kwon, Heedoo Lee, Seok Kim, Young Tae Cho
The sustained water repellency of interconnected micropatterned surfaces is explored over an extended duration, with a focus on their resilience during a 90‐day water‐immersion test. Initially, the microstructure surfaces exhibit high water repellency, a characteristic of the Cassie–Baxter state. However, subsequent detailed temporal analyses reveal varying responses depending on the structural topology. The interconnected micropatterned surfaces exhibit remarkable long‐term resistance to water; this is attributed to the formation of large and stable air pockets enabled by their unique microcavity structures. In comparison, hierarchical microcavity surfaces with micropillars exhibit a notable decrease in water repellency, as evidenced by reduced contact angles, suggesting a transition to a wetting state owing to the emergence of surface hydrophilicity during long‐term water exposure. This study demonstrates the importance of stable air‐pocket effects, particularly in applications where the long‐term stability of liquid repellency is critical, and suggests the role of interconnected structures in maintaining water repellency over time.
本研究探讨了相互连接的微图案表面在较长时间内的持续憎水性,重点是其在 90 天浸水试验中的韧性。最初,微结构表面表现出很高的憎水性,这是卡西-巴克斯特状态的一个特征。然而,随后的详细时间分析表明,不同的结构拓扑会产生不同的反应。相互连接的微图案表面表现出显著的长期拒水性;这归因于其独特的微腔结构形成了大而稳定的气穴。相比之下,带有微柱的分层微腔表面的憎水性明显下降,接触角减小就是证明,这表明在长期接触水的过程中,由于表面亲水性的出现而过渡到了润湿状态。这项研究证明了稳定的气穴效应的重要性,尤其是在对憎液性的长期稳定性要求极高的应用领域,同时也表明了相互连接的结构在长期保持憎水性方面的作用。
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引用次数: 0
UV to NIR Broadband Flexible Photodetector Based on Solution-Processed MoS2/PDPP3T Inorganic–Organic Hybrid Heterostructures 基于溶液加工 MoS2/PDPP3T 无机有机杂化异质结构的紫外至近红外宽带柔性光电探测器
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-04-28 DOI: 10.1002/admi.202301065
Daxiu Tang, Zhenyu Du, Ying Xie, Feiyu Zhao, Xiangdong Yang, Chenjie Gu, Xiang Shen

Molybdenum disulfide (MoS2) is a 2D material with excellent electrical and optical properties, and developing a universal technology for the preparation of high-performance MoS2-based photodetector is extremely desirable. Here, a UV to NIR broadband flexible photodetector based on MoS2/(PDPP3T) inorganic–organic hybrid heterostructures is reported. In the experiment, high crystalline 2H-phase few-layer MoS2 nanoflakes are first prepared by optimized electrochemical intercalation of tetraheptylammonium cation (THA+) and ultrasound-assisted exfoliation strategy. Thereafter, a narrow bandgap organic semiconductor PDPP3T is introduced to construct the MoS2/Poly(diketopyrrolopyrrolothiophrn) (PDPP3T) heterojunction. Experimental results reveal that the photodetector can have broadband photo response from 380 to 980 nm. Meanwhile, excellent responsivities and detectivity of 12.4 mA W−1, 2.2 × 1010 Jones at 380 nm and 0.1 mA W−1 and 5 × 108 Jones at 980 nm are achieved, which are ≈10 (UV band)/100 (NIR band) times high than that obtained on the pure MoS2-based detector. Moreover, the flexibility of the device is investigated by conformal covering the device on a curved surface (R = 5 and 2.5 mm), it shows that the photo response remains almost the same as that measured on the planar substrate, indicating the possible application in the wearable electronics.

二硫化钼(MoS2)是一种二维材料,具有优异的电学和光学性能,因此开发一种通用技术来制备基于 MoS2 的高性能光电探测器是非常有必要的。本文报道了一种基于 MoS2/(PDPP3T)无机有机杂化异质结构的紫外至近红外宽带柔性光探测器。实验中,首先通过优化的电化学插层四庚基铵阳离子(THA+)和超声辅助剥离策略制备了高结晶的 2H 相少层 MoS2 纳米片。之后,引入窄带隙有机半导体 PDPP3T 构建 MoS2/Poly(diketopyrrolopyrrolothiophrn) (PDPP3T) 异质结。实验结果表明,该光电探测器具有 380 至 980 纳米的宽带光响应。同时,在 380 纳米波段实现了 12.4 mA W-1 和 2.2 × 1010 琼斯的优异响应度和探测度,在 980 纳米波段实现了 0.1 mA W-1 和 5 × 108 琼斯的优异响应度和探测度,是纯 MoS2 基探测器的 10 倍(紫外波段)/100 倍(近红外波段)。此外,通过在弯曲表面(R = 5 和 2.5 毫米)上保形覆盖该器件,研究了该器件的灵活性,结果表明光响应与在平面基底上测得的光响应几乎相同,这表明该器件有可能应用于可穿戴电子设备。
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引用次数: 0
Nitrogen Doping in VO2 Thin Films on Synthetic Mica Substrates Through Mist Chemical Vapor Deposition: Lowering the Metal–Insulator Transition Temperature Toward Smart Windows 通过喷雾化学气相沉积在合成云母基底上的 VO2 薄膜中掺氮:降低金属-绝缘体转变温度,实现智能窗口
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-04-26 DOI: 10.1002/admi.202400038
Taisei Kano, Hiroyuki Nishinaka, Yuta Arata, Masahiro Yoshimoto
In this study, nitrogen (N) is doped into VO2 thin films through mist chemical vapor deposition (CVD), and the effect of the doping on metal–insulator transition (MIT) temperatures is investigated. The N‐doped VO2 thin films are grown on an SnO2 buffer layer. The N‐doped VO2 lattice spacing tends to expand as the growth temperature decreased, which indicates that the incorporation of N into the lattice is derived from the Ethylenediamine. Secondary ion mass spectrometry (SIMS) is conducted to investigate the relationship between the decrease in the transition temperature and N concentration. The results reveal that the sample grown at 425 °C contains approximately 2 × 1020 cm−3 of N. Thus, efficient nitrogen doping can be achieved through mist CVD. The temperature‐resistance characteristics of VO2 thin films are measured to investigate their electrical properties and MIT temperatures. The results reveal that for undoped samples, the transition temperature slightly decreases with the decrease in the growth temperature. Furthermore, the sample grown at 425 °C exhibits a considerable change in resistance because of MIT at approximately 29.5 °C. These results prove the potential of using mist CVD N‐doped thin films for smart window applications to address future energy problems.
本研究通过雾化化学气相沉积(CVD)将氮(N)掺杂到 VO2 薄膜中,并研究了掺杂对金属-绝缘体转变(MIT)温度的影响。掺杂 N 的 VO2 薄膜生长在 SnO2 缓冲层上。随着生长温度的降低,掺 N 的 VO2 晶格间距趋于扩大,这表明 N 在晶格中的掺入来自乙二胺。二次离子质谱法(SIMS)用于研究转变温度的降低与 N 浓度之间的关系。结果表明,在 425 °C 生长的样品含有约 2 × 1020 cm-3 的 N。测量了 VO2 薄膜的温度-电阻特性,以研究其电气特性和 MIT 温度。结果表明,对于未掺杂的样品,转变温度随着生长温度的降低而略有降低。此外,生长温度为 425 ℃ 的样品在大约 29.5 ℃ 时会出现 MIT,从而导致电阻发生显著变化。这些结果证明了将雾状 CVD 掺杂 N 薄膜用于智能窗应用以解决未来能源问题的潜力。
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引用次数: 0
Manufacturing Free-Standing, Porous Metallic Layers with Dynamic Hydrogen Bubble Templating 利用动态氢气泡模板制造独立多孔金属层
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-04-25 DOI: 10.1002/admi.202400052
Adrian Mularczyk, Daniel Niblett, Adam Wijpkema, Marc P. F. H. L. van Maris, Antoni Forner-Cuenca

The 3D structure (i.e., microstructure) of porous electrodes governs the performance of emerging electrochemical technologies such as fuel cells, electrolysis, and batteries. Sustaining electrochemical reactions and convective-diffusive mass transport at high efficiency is complex and motivates the search for sophisticated microstructures with multimodal pore size distributions and pore size gradients. Here a new synthesis route for porous, metallic layers is presented that combines the characteristics of carbon structures (i.e., pore size, porosity) with the properties of metals (i.e., recyclability, conductivity). Building on the method of dynamic hydrogen bubble templating, a novel approach is engineered to manufacture thin, free-standing layers using an electrochemical flow cell through the introduction of an intermediate layer and optimization of the synthesis parameters. Mechanically stable layers are created with thicknesses ranging from ≈50 to ≈200 µm comprising porous, dendritic structures, arranged to form a vascular network of larger pores with a gradient in radii from ≈5 µm at the bottom and up to ≈36 µm at the top of the material. Using X-ray tomographic data, the morphology is analyzed, and the diffusive transport through the material as a function of liquid filling is simulated and compared to state-of-the-art carbon fiber-based electrodes, showing significantly higher mass transfer properties.

多孔电极的三维结构(即微结构)决定着燃料电池、电解和电池等新兴电化学技术的性能。维持高效率的电化学反应和对流扩散质量传输非常复杂,因此需要寻找具有多模态孔径分布和孔径梯度的复杂微结构。本文介绍了一种新的多孔金属层合成路线,它结合了碳结构的特点(如孔径、孔隙率)和金属的特性(如可回收性、导电性)。在动态氢气泡模板法的基础上,通过引入中间层和优化合成参数,设计出一种利用电化学流动池制造独立薄层的新方法。制造出的机械稳定层厚度从 ≈50 微米到 ≈200 微米不等,由多孔树枝状结构组成,排列成由较大孔隙组成的血管网络,半径梯度从材料底部的 ≈5 微米到顶部的 ≈36 微米不等。利用 X 射线层析成像数据对其形态进行了分析,模拟了作为液体填充函数的材料扩散传输,并与最先进的碳纤维电极进行了比较,结果表明其传质性能明显更高。
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引用次数: 0
Masthead: (Adv. Mater. Interfaces 12/2024) 刊头:(Adv. Mater. Interfaces 12/2024)
IF 5.4 3区 材料科学 Q1 Engineering Pub Date : 2024-04-24 DOI: 10.1002/admi.202470034
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引用次数: 0
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