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The Anti/Deicing Performance of the Low Interfacial Toughness Coating Is Enhanced: Induced Ice Crack Generation and Its Extension. 增强低界面韧性涂层的防除冰性能:诱导冰裂纹的产生及其扩展。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 Epub Date: 2024-11-05 DOI: 10.1021/acs.langmuir.4c03672
Senyun Liu, Lingfeng Zhao, Bingquan Wu, Yizhou Shen, Weilan Liu, Junjian He

The low interfacial toughness of the material surface is important for crack initiation and expansion of the ice layer as it remains an effective method for large-scale deicing. However, there are challenges, such as a large critical icing size and incomplete shedding of the ice layer. Adjusting the interfacial forces to make the ice more prone to cracking, expanding, and shedding is advantageous in addressing the problem of anti-icing failure in materials with low interfacial toughness. Therefore, we propose a deicing strategy that combines porous PDMS (polydimethylsiloxane) coatings with low interfacial toughness and piezoelectric vibration. A series of hydrophobic porous PDMS coatings with different porosities were prepared on the surface of an aluminum alloy substrate through curing and phase separation. The elastic modulus of the coatings decreased from 1465 to 509 kPa as the coating porosity increased, revealing the mechanism behind the improvement in mechanical properties. The key to promoting ice fracture on porous PDMS coatings lies in the synergistic effect of the out-of-plane shear stress and microcracks at the solid-ice interface. This work focuses on exploring the characteristics of interfacial forces by combining the intrinsic mechanical properties of coatings with external forces, providing new insights for designing low interfacial toughness anti-icing materials.

材料表面的界面韧性较低,这对冰层的开裂和扩展非常重要,因为它仍然是大规模除冰的有效方法。但也存在一些挑战,如临界结冰尺寸大、冰层脱落不完全等。调整界面力使冰层更容易开裂、膨胀和脱落,有利于解决界面韧性低的材料的防冰失效问题。因此,我们提出了一种将具有低界面韧性的多孔 PDMS(聚二甲基硅氧烷)涂层与压电振动相结合的除冰策略。通过固化和相分离,在铝合金基材表面制备了一系列具有不同孔隙率的疏水多孔 PDMS 涂层。随着涂层孔隙率的增加,涂层的弹性模量从 1465 kPa 下降到 509 kPa,揭示了机械性能改善背后的机理。促进多孔 PDMS 涂层上冰断裂的关键在于平面外剪切应力和固冰界面微裂缝的协同效应。这项工作的重点是通过将涂层的内在力学性能与外力相结合来探索界面力的特性,为设计低界面韧性的防冰材料提供新的见解。
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引用次数: 0
Competing Bifurcations Determine Symmetry Breaking During Droplet Snaps on Smooth Patterned Surfaces. 竞争性分岔决定了光滑图案表面水滴扣合过程中的对称性破坏。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 Epub Date: 2024-11-06 DOI: 10.1021/acs.langmuir.4c02908
Lucile Bisquert, Élfego Ruiz-Gutiérrez, Marc Pradas, Rodrigo Ledesma-Aguilar

The shape and stability of a droplet in contact with a solid surface is affected by the chemical composition and topography of the solid, and crucially, by the droplet's size. During a variation in size, most often observed during evaporation, droplets on smooth patterned surfaces can undergo sudden shape and position changes. Such changes, called snaps, are prompted by the surface pattern and arise from fold and pitchfork bifurcations which respectively cause symmetric and asymmetric motions. Yet, which type of snap is likely to be observed is an open fundamental question that has relevance in the rational design of surfaces for managing droplets. Here we show that the likelihood of observing symmetric or asymmetric snaps depends on the distance between fold and pitchfork bifurcation points and on how this distance varies for droplets that grow or shrink in size on surfaces patterned with a smooth topography. Our results can help develop strategies to control droplets by exploiting smooth surface patterns but also have broader relevance in situations where different types of bifurcations compete in determining the stability of a system, for instance in snap-through instabilities observed in elastic media.

与固体表面接触的液滴的形状和稳定性受固体的化学成分和地形的影响,最重要的是受液滴大小的影响。在蒸发过程中最常观察到的尺寸变化过程中,光滑图案表面上的液滴会发生形状和位置的突然变化。这种变化被称为 "突变"(snap),是由表面图案引起的,由分别引起对称和不对称运动的褶皱和杈状分叉产生。然而,哪种类型的卡扣有可能被观察到是一个未决的基本问题,它与管理液滴的表面的合理设计息息相关。在这里,我们展示了观察到对称或不对称卡扣的可能性取决于折叠点和叉形分叉点之间的距离,以及液滴在具有光滑地形图案的表面上增大或缩小时这一距离的变化情况。我们的研究结果不仅有助于开发利用光滑表面图案控制液滴的策略,而且在不同类型的分叉竞争决定系统稳定性的情况下,例如在弹性介质中观察到的卡突不稳定性中,也具有更广泛的意义。
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引用次数: 0
Controllable Structure Design of an Organic Gel-Infused Porous Surface for Efficient Anti- and De-icing 用于高效防冰和除冰的有机凝胶注入式多孔表面的可控结构设计
IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1021/acs.langmuir.4c04110
Weiming Lin, Haonan Song, Huimin Qi, Xingshi Gu, Ding Zhang, Jiaxin Yu, Yafeng Zhang, Gai Zhao
Icing causes many problems in daily life and with equipment stability, and many efforts have been made to remove surface icing. Herein, a novel organic gel-infused porous material is developed to achieve excellent de-icing performance. Porous polydimethylsiloxane (P-PDMS) composites with different pore sizes were prepared by a template method. The two-phase skeletons and/or gel material was obtained by infusing PDMS gel into P-PDMS (GIP-PDMS). The ice adhesion strength of GIP-PDMS under static and dynamic icing conditions was comparatively investigated. The results show that GIP-PDMS displayed excellent anti-icing performance, and the delay freezing time of GIP-PDMS1 was ∼4554 s at −5 °C. The ice adhesion strength of GIP-PDMS was much lower than that of P-PDMS, owing to the distinct modulus between the two-phase skeletons and/or gel. The simulation results indicated that the stress concentration promoted ice fracture and contributed to weak ice adhesion. Molecular dynamics further showed that the state of the molecular chains and the interfacial interaction between ice and PDMS gel at 268 K helped to decrease the shear force.
结冰给日常生活和设备稳定性带来了许多问题,人们为消除表面结冰付出了许多努力。本文开发了一种新型有机凝胶注入多孔材料,以实现优异的除冰性能。采用模板法制备了不同孔径的多孔聚二甲基硅氧烷(P-PDMS)复合材料。通过将 PDMS 凝胶注入 P-PDMS (GIP-PDMS),获得了两相骨架和/或凝胶材料。比较研究了 GIP-PDMS 在静态和动态结冰条件下的冰粘附强度。结果表明,GIP-PDMS 具有优异的抗冰性能,GIP-PDMS1 在-5 °C时的延迟冻结时间为 4554 s。由于两相骨架和/或凝胶之间的模量不同,GIP-PDMS 的附冰强度远低于 P-PDMS。模拟结果表明,应力集中促进了冰的断裂,并导致冰的粘附力减弱。分子动力学进一步表明,分子链的状态以及在 268 K 下冰与 PDMS 凝胶之间的界面相互作用有助于降低剪切力。
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引用次数: 0
Fe-Doped Ni3S2 Induces Self-Reconstruction for Urea-Assisted Water Electrolysis Enhancement. 掺铁 Ni3S2 可诱导尿素辅助水电解增强的自重构。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 Epub Date: 2024-11-06 DOI: 10.1021/acs.langmuir.4c03343
Xinyu Yang, Yifeng Liu, Qianqiao Chen, Wanchin Yu, Qin Zhong

Urea oxidation reaction (UOR) is an attractive alternative anodic reaction to oxygen evolution reaction (OER) for its low thermodynamic potential (0.37 V vs RHE). A major challenge that prohibits its practical application is the six-electron transfer process during UOR, demanding enhancements in the catalytic activity. Herein, a Fe-doped Ni3S2 catalyst with a uniform flower-like structure is synthesized in situ on nickel foam via a simple one-step hydrothermal method. The electrochemical properties of Fe-Ni3S2 are significantly improved since a current density of 10 mA cm-2 only requires a 1.33 V potential and remains stable for 60 h. The structural characterization demonstrates a strong interaction between Fe and Ni3S2. After Fe doping, the active site increases, which promotes the formation of NiOOH on the catalyst surface, thus speeding up the UOR process. These changes are beneficial to charge transfer and optimize the adsorption energy of the intermediates. In situ EIS further confirms that Fe promotes electron transfer during the UOR process, reduces the interface resistance between the catalyst and the electrolyte, and lowers the driving voltage.

尿素氧化反应(UOR)的热力学电位较低(0.37 V 对 RHE),是氧进化反应(OER)的一种有吸引力的替代阳极反应。阻碍其实际应用的一个主要挑战是 UOR 反应过程中的六电子转移过程,这就要求提高催化活性。本文通过简单的一步水热法,在泡沫镍上原位合成了具有均匀花状结构的掺铁 Ni3S2 催化剂。由于 10 mA cm-2 的电流密度只需要 1.33 V 的电位,且能保持稳定 60 小时,Fe-Ni3S2 的电化学性能得到了显著改善。掺入 Fe 后,活性位点增加,促进了催化剂表面 NiOOH 的形成,从而加快了 UOR 过程。这些变化有利于电荷转移,并优化了中间产物的吸附能。原位 EIS 进一步证实,铁在 UOR 过程中促进了电子转移,降低了催化剂与电解质之间的界面电阻,并降低了驱动电压。
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引用次数: 0
Zwitterion-Conjugated Protein Coatings for Enhanced Antifouling in Complex Biofluids: Underlying Molecular Interaction Mechanisms. 用于在复杂生物流体中增强防污能力的齐聚物共轭蛋白涂层:基本分子相互作用机制。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1021/acs.langmuir.4c03975
Ziqian Zhao, Charley Huang, Hongbo Zeng

Biofouling can cause severe infections, device malfunctions, and failures in diagnostics and therapeutics. Proteins such as bovine serum albumin (BSA) have recently been used as coatings to resist biofouling because they combine surface anchoring and antifouling properties. However, their antifouling effectiveness will significantly deteriorate in complex biofluids with high salinity, limiting their practical applications. In this work, we developed a zwitterion-conjugated protein with enhanced antifouling capability by grafting zwitterionic 2-methacryloyloxyethyl phosphorylcholine (MPC) onto BSA protein via a click reaction. This conjugated protein can easily anchor on various substrates, both inorganic and organic, and exhibits efficient and broad-spectrum fouling resistance to metabolites, proteins, and complex biofluids. Even in the complex fetal bovine serum with higher salinity, the BSA@MPC coating can also maintain 99% fouling resistance robustly, over 6-fold superior to native BSA-coated surfaces in antifouling capability. Direct surface forces measurement reveals that such outstanding antifouling properties of conjugated protein BSA@MPC could be attributed to the stable hydration layer on its surface and the steric repulsion from the antipolyelectrolyte behavior of zwitterionic MPC polymer in the high-salinity environment. Our findings advance the development of protein-based functional materials and provide valuable insights for designing novel antifouling surfaces for marine, food, and bioengineering applications.

生物污垢可导致严重感染、设备故障以及诊断和治疗失败。牛血清白蛋白(BSA)等蛋白质兼具表面锚定和防污特性,最近被用作抗生物污染的涂层。然而,在高盐度的复杂生物流体中,它们的防污效果会明显下降,从而限制了它们的实际应用。在这项研究中,我们通过单击反应,在 BSA 蛋白上接枝了齐聚物 2-甲基丙烯酰氧乙基磷酰胆碱(MPC),从而开发出了一种具有更强防污能力的齐聚物共轭蛋白。这种共轭蛋白可轻松锚定在各种无机和有机基质上,并对代谢物、蛋白质和复杂的生物流体表现出高效、广谱的防污能力。即使在盐度较高的复杂胎牛血清中,BSA@MPC 涂层也能保持 99% 的抗污能力,在抗污能力方面比原生 BSA 涂层表面高出 6 倍以上。直接的表面力测量结果表明,共轭蛋白质 BSA@MPC 具有如此出色的防污性能,可能是由于其表面具有稳定的水合层,以及在高盐度环境中,齐聚物 MPC 聚合物的抗偶电解质行为产生了立体排斥。我们的研究结果推动了基于蛋白质的功能材料的发展,并为设计海洋、食品和生物工程应用领域的新型防污表面提供了宝贵的见解。
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引用次数: 0
In Situ Stabilization of Bi Nanoparticles into the Nanopores of Modified Montmorillonite: Efficient Heterogeneous Catalysts for Reduction of 4-Nitrophenol. 将生物纳米颗粒原位稳定到改性蒙脱石的纳米孔中:用于还原 4-硝基苯酚的高效异相催化剂。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 Epub Date: 2024-11-04 DOI: 10.1021/acs.langmuir.4c02477
Utpal Sadhonider, Jayashree Nath, Gitashree Darabdhara, Arabinda Baruah, Lakshi Saikia, Bhaskar Jyoti Sarmah

Here, we report the in situ generation of Bi nanoparticles (BiNPs) into a nanoporous matrix by impregnation of bismuth chloride and subsequent reduction with sodium borohydride. The nanoporous matrix was created by acid activation of natural montmorillonite clay under controlled conditions with the aim that it may serve as a host for BiNPs. The characterization of stabilized BiNPs was done by using Fourier-transform infrared (FTIR), powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), transmission electron microscopy (TEM), and field emission scanning electron microscopy-energy dispersive X-ray (FESEM-EDX) techniques. The TEM study reveals that the BiNPs with an average particle size of 7.16 nm are well-distributed on the surface of the acid-activated montmorillonite clay. The synthesized BiNPs exhibited excellent catalytic activity for the degradation of 4-nitrophenol (4-NP) in aqueous medium with remarkable results. The degradation of 4-NP to 4-aminophenol (4-AP) at 25 °C, in the presence of sodium borohydride, brought about almost 100% conversion in 6 min with a rate constant of 0.20098 s-1 that follows the pseudo-first-order kinetics.

在此,我们报告了通过浸渍氯化铋并随后用硼氢化钠还原,在纳米多孔基质中原位生成生物纳米粒子(BiNPs)的过程。这种纳米多孔基质是在受控条件下通过酸活化天然蒙脱石粘土而形成的,目的是使其成为生物纳米粒子的宿主。使用傅立叶变换红外(FTIR)、粉末 X 射线衍射(PXRD)、X 射线光电子能谱(XPS)、热重分析(TGA)、透射电子显微镜(TEM)和场发射扫描电子显微镜-能量色散 X 射线(FESEM-EDX)技术对稳定的 BiNPs 进行了表征。TEM 研究表明,平均粒径为 7.16 nm 的 BiNPs 在酸活化蒙脱石粘土表面分布均匀。合成的 BiNPs 在水介质中降解 4-硝基苯酚(4-NP)时表现出优异的催化活性,效果显著。在硼氢化钠存在下,4-NP 在 25 ℃ 下降解为 4-氨基苯酚(4-AP),6 分钟内的转化率几乎达到 100%,速率常数为 0.20098 s-1,遵循伪一阶动力学。
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引用次数: 0
Recent Advances in Immobilizing and Benchmarking Molecular Catalysts for Artificial Photosynthesis. 人工光合作用分子催化剂固定化和基准研究的最新进展。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 Epub Date: 2024-11-04 DOI: 10.1021/acs.langmuir.4c03249
Lei Wang, Mengjiao Shao, Zhu-Lin Xie, Karen L Mulfort

Transition metal complexes have been widely used as catalysts or chromophores in artificial photosynthesis. Traditionally, they are employed in homogeneous settings. Despite their functional versatility and structural tunability, broad industrial applications of these catalysts are impeded by the limitations of homogeneous catalysis such as poor catalyst recyclability, solvent constraints (mostly organic solvents), and catalyst durability. Over the past few decades, researchers have developed various methods for molecular catalyst heterogenization to overcome these limitations. In this review, we summarize recent developments in heterogenization strategies, with a focus on describing methods employed in the heterogenization process and their effects on catalytic performances. Alongside the in-depth discussion of heterogenization strategies, this review aims to provide a concise overview of the key metrics associated with heterogenized systems. We hope this review will aid researchers who are new to this research field in gaining a better understanding.

过渡金属复合物已被广泛用作人工光合作用的催化剂或发色团。传统上,它们是在均相环境中使用的。尽管这些催化剂具有功能多样性和结构可调性,但其广泛的工业应用受到均相催化的限制,如催化剂可回收性差、溶剂限制(主要是有机溶剂)和催化剂耐久性等。在过去几十年中,研究人员开发了各种分子催化剂异质化方法,以克服这些局限性。在本综述中,我们总结了异质化策略的最新发展,重点介绍了异质化过程中采用的方法及其对催化性能的影响。在深入讨论异质化策略的同时,本综述还旨在简要概述与异质化系统相关的关键指标。我们希望这篇综述能帮助初涉这一研究领域的研究人员更好地了解这一领域。
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引用次数: 0
Enhancing Internal Electric Field of Metal-Free Donor-Acceptor Conjugated Photocatalysts for Efficient Photocatalytic Degradation of Tetracycline and CO2 Reduction. 增强无金属供体-受体共轭光催化剂的内电场以实现四环素的高效光催化降解和二氧化碳还原
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1021/acs.langmuir.4c03632
Guangyu Wu, Geng Li, Yonggong Tang, Guoyu Tai, Yuwei Pan, Jiangang Han, Weinan Xing

Constructing alternating donor-acceptor (D-A) units within g-C3N4 represents an effective strategy for enhancing photocatalytic performance through improved charge carrier separation while concurrently addressing energy shortages and facilitating wastewater remediation. Here, a series of D-A-type conjugated photocatalysts (CNBTC-X) are prepared using g-C3N4 as an acceptor unit and different masses of 5-bromo-2-thiophenecarboxaldehyde (BTC) as a donor unit by a one-step thermal polymerization. CNBTC-50 presents higher photocatalytic properties for CO2 reduction coupled with tetracycline (TC) removal than those of g-C3N4, CNBTC-10, CNBTC-30, and CNBTC-70. The introduction of the unique electron-donor-acceptor structure effectively drives the separation and transfer of photoinduced carriers while reducing the internal carrier transfer hindrance. Photocatalytic experiments reveal that the CNBTC-50 photocatalyst achieves up to 94.6% TC removal under visible light irradiation conditions. Compared with that of the pristine g-C3N4, the photocatalytic degradation reaction rate constant of CNBTC-50 is significantly increased by about 3.87 times. The study examines the influence of various reaction parameters on degradation activity, including catalyst concentration, pH, and TC concentration. Additionally, LC-MS is utilized to perform a comprehensive analysis of the intermediates and pathways involved in TC degradation. Furthermore, CNBTC-50 demonstrates remarkable photocatalytic CO2 reduction activity, achieving rates of 20.83 μmol g-1 h-1 (CO) and 9.36 μmol g-1 h-1 (CH4), which are 10.68 and 5.98 times more efficient than those of g-C3N4, respectively. This work aims to offer valuable guidance for the rational design of nonmetal D-A-structured catalysts and effectively integrates reaction systems to couple CO2 reduction with antibiotic removal.

在 g-C3N4 中构建交替的供体-受体(D-A)单元是通过改善电荷载流子分离来提高光催化性能的有效策略,同时还能解决能源短缺问题并促进废水修复。本文以 g-C3N4 为受体单元,以不同质量的 5-溴-2-噻吩甲醛(BTC)为供体单元,通过一步热聚合法制备了一系列 D-A 型共轭光催化剂(CNBTC-X)。与 g-C3N4、CNBTC-10、CNBTC-30 和 CNBTC-70 相比,CNBTC-50 在二氧化碳还原和四环素(TC)去除方面具有更高的光催化性能。独特的电子-供体-受体结构的引入有效地促进了光诱导载流子的分离和转移,同时减少了内部载流子的转移阻碍。光催化实验表明,在可见光照射条件下,CNBTC-50 光催化剂的三氯甲烷去除率高达 94.6%。与原始 g-C3N4 相比,CNBTC-50 的光催化降解反应速率常数显著提高了约 3.87 倍。研究考察了催化剂浓度、pH 值和 TC 浓度等各种反应参数对降解活性的影响。此外,还利用 LC-MS 对 TC 降解过程中的中间产物和途径进行了全面分析。此外,CNBTC-50 还表现出显著的光催化二氧化碳还原活性,其还原速率分别达到 20.83 μmol g-1 h-1 (CO)和 9.36 μmol g-1 h-1 (CH4),分别是 g-C3N4 的 10.68 倍和 5.98 倍。这项工作旨在为合理设计非金属 D-A 结构催化剂提供有价值的指导,并有效整合反应体系,将二氧化碳还原与抗生素去除结合起来。
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引用次数: 0
Effects of Thermal Energy on the Formation of Lattice Strain in VO2 Thin Films Grown on TiO2(001). 热能对在 TiO2(001) 上生长的 VO2 薄膜中形成晶格应变的影响。
IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 Epub Date: 2024-11-06 DOI: 10.1021/acs.langmuir.4c03004
Reki Nakamoto, Hiroyuki Okazaki, Takanori Wakita, Takayoshi Yokoya, Yuji Muraoka

Film thickness is a well-known experimental parameter for controlling lattice strain in oxide films. However, due to environmental and resource conservation considerations, films need to be as thin as possible, increasing the need to find alternative factors for strain management. Herein, we present the importance of thermal energy as a factor for the formation of lattice strain in the oxide films, specifically focusing on the effects of laser fluence during pulsed laser deposition (PLD) on the in-plane lattice strain of vanadium dioxide (VO2) thin films grown on titanium dioxide (TiO2) (001). VO2 thin films were deposited using a KrF excimer laser (λ = 248 nm) at laser fluences ranging from 0.88 to 1.70 J/cm2. The film thickness ranged from 10-15 nm, below the critical thickness. Films grown at higher laser fluences exhibited smooth surfaces and completely strained in-plane lattices. In contrast, films grown at lower laser fluences displayed numerous small islands and relaxed in-plane lattice strain. The metal-insulator transition (MIT) temperature was lower for films grown at higher laser fluencies compared to those grown at lower laser fluences. It was also revealed that Ti-V interdiffusion occurs, forming a solid solution (V1-xTixO2) near the interface. These observations suggest that the thermal energy of the particles, influenced by laser fluence, is a critical factor in the formation of lattice strain in metal oxide films and also that laser fluence in PLD is an effective experimental parameter for strain management in oxide films. Our findings enhance the understanding of lattice strain formation in metal oxides and offer insights for establishing effective methods for controlling lattice strain in metal oxide films.

薄膜厚度是众所周知的控制氧化物薄膜晶格应变的实验参数。然而,出于环境和资源保护的考虑,薄膜需要越薄越好,这就更需要找到应变管理的替代因素。在此,我们介绍了热能作为氧化物薄膜晶格应变形成的一个重要因素,特别是脉冲激光沉积(PLD)过程中激光通量对生长在二氧化钛(TiO2)(001)上的二氧化钒(VO2)薄膜面内晶格应变的影响。VO2 薄膜使用 KrF 准分子激光器(λ = 248 nm)在 0.88 至 1.70 J/cm2 的激光通量下沉积。薄膜厚度为 10-15 nm,低于临界厚度。在较高激光通量下生长的薄膜表面光滑,面内晶格完全紧张。与此相反,在较低激光通量下生长的薄膜则显示出许多小的孤岛和松弛的面内晶格应变。与低激光通量下生长的薄膜相比,高激光通量下生长的薄膜的金属-绝缘体转变(MIT)温度更低。研究还发现,Ti-V 发生了相互扩散,在界面附近形成了固溶体(V1-xTixO2)。这些观察结果表明,粒子的热能受激光通量的影响,是金属氧化物薄膜中形成晶格应变的关键因素,而且 PLD 中的激光通量是氧化物薄膜应变管理的有效实验参数。我们的发现加深了人们对金属氧化物晶格应变形成的理解,并为建立控制金属氧化物薄膜晶格应变的有效方法提供了启示。
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引用次数: 0
Discontinuous Directional Wetting Transitions in Polymeric Droplets on the Heterogeneous Microcavity Surface 异质微腔表面上聚合物液滴的不连续定向润湿转变
IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-19 DOI: 10.1021/acs.langmuir.4c03024
Wenshuai Xu, Kuo Yan, Lingling Zhao, Yifan He, Heng Jiang, Yonggang Min
The wetting transition behaviors of polymeric droplets on microcavity surfaces are familiar and play a vital role in micromanufacturing, microfluidics, and printing industries. Despite previous research indicating that microcavity surfaces can precisely control the droplet wetting state, the understanding of the complex effects of droplet spreading, surface morphology, and property of polymeric droplet on wetting transitions remains incomplete. The air–liquid interfaces (ALIs) typically arise from the entrapped air beneath the droplet on microcavity surfaces, adopting a metastable wetting state caused by either bubble escape or dissolution. Here, we discovered a previously unobserved phenomenon: the time-dependent evolution of regularly arranged ALIs with discontinuous wetting states, along with the pronounced directional wetting transitions from the Cassie–Baxter state to the Wenzel state upon deposition of polymeric droplets on heterogeneous microcavity surfaces. The durability of ALIs in microcavities was quantified, illustrating that the wetting transitions associated with droplet spreading processes obeyed power laws. By integrating the wetting theory and the viscoelastic effect of polymeric droplet, we have proposed a phenomenological coevolution model for wetting transitions that emphasizes the synergistic interaction between adjacent microcavities, resulting in the observed cluster evolution behavior of ALIs within droplets. Our study holds great significance in guiding soft manufacturing techniques utilizing internal ALIs as templates. The established mechanism opens up avenues for investigating the intricate wetting phenomena of polymeric droplets on microtextured substrates.
聚合物液滴在微腔表面上的润湿转换行为已为人们所熟知,并在微制造、微流体和印刷行业中发挥着重要作用。尽管之前的研究表明微腔表面可以精确控制液滴的润湿状态,但人们对液滴扩散、表面形态和聚合物液滴性质对润湿转变的复杂影响的理解仍不全面。气液界面(ALIs)通常产生于微腔表面液滴下方的夹带空气,由于气泡逸出或溶解而形成一种可变的润湿状态。在这里,我们发现了一个以前从未观察到的现象:当聚合物液滴沉积在异质微腔表面时,具有不连续润湿状态的有规则排列的 ALI 随时间发生演变,并从卡西-巴克斯特状态向文泽尔状态发生明显的定向润湿转变。对微腔中 ALI 的持久性进行了量化,表明与液滴扩散过程相关的润湿转变服从幂律。通过整合润湿理论和聚合物液滴的粘弹性效应,我们提出了润湿转换的现象学协同演化模型,该模型强调了相邻微腔之间的协同作用,从而观察到液滴内 ALIs 的集群演化行为。我们的研究对于指导利用内部 ALIs 作为模板的软制造技术具有重要意义。所建立的机制为研究聚合物液滴在微纹理基底上错综复杂的润湿现象开辟了途径。
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