Surfaces and Interfaces最新文献_第4页

Femtosecond laser-induced plasma-assisted backward deposition of robustly adherent porous carbon films on glass substrates 飞秒激光诱导等离子体辅助在玻璃基底上反向沉积牢固附着的多孔碳薄膜

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105304

Sheng Peng , Junjie Zou , Tangyang Pu , Heng Wang , Ruonan Wang , Xiaoyu Tian , Sheng Liu , Qiang Cao

The simple and rapid production and transfer of high-quality carbon materials are crucial for the flexible and efficient fabrication of carbon-based electronic devices. Recently, a laser-assisted transfer method combining laser-induced carbonization and transfer printing was demonstrated for the one-step preparation and transfer of patterned laser-induced carbon films to transparent substrates. However, this method is limited by insufficient robustness and weak adhesion of the carbon film post-transfer. Herein, we developed a non-contact laser-induced plasma-assisted deposition method to deposit robustly adherent porous carbon films on glass substrates. By well-adjusting the laser parameters and inserting spacers with adjustable thickness, laser-induced plasma ablation replaced direct laser ablation during femtosecond laser scanning of the substrate-polyimide-carrier sandwich structure, resulting in micro-channels with a carbon-glass recast layer instead of easily peelable flakes on the glass substrate. This hierarchical structure significantly enhances the adhesion between the laser-induced carbon film and the glass substrate, ensuring outstanding stability of the deposited carbon film under various adhesion tests. Furthermore, compared to carbon films prepared by the laser-assisted transfer method, the obtained carbon films are hydrophilic, low-resistance, and porous, facilitating the fabrication of energy storage devices. To demonstrate its practical application, a planar carbon-based micro-supercapacitor was fabricated on glass, exhibiting excellent electrochemical and cycling performance.

简单快速地生产和转移高质量的碳材料对于灵活高效地制造碳基电子器件至关重要。最近，一种结合了激光诱导碳化和转印的激光辅助转印方法被证明可一步制备激光诱导碳膜图案并将其转印到透明基底上。然而，这种方法受限于碳膜的不稳定性和转移后的弱附着力。在此，我们开发了一种非接触式激光诱导等离子体辅助沉积方法，可在玻璃基底上沉积牢固附着的多孔碳膜。在飞秒激光扫描基底-聚酰亚胺-载体夹层结构的过程中，通过精心调整激光参数和插入厚度可调的间隔物，激光诱导等离子体烧蚀取代了直接激光烧蚀，从而在玻璃基底上形成具有碳-玻璃重铸层的微通道，而不是容易剥离的薄片。这种分层结构大大增强了激光诱导碳膜与玻璃基底之间的粘附力，确保了沉积碳膜在各种粘附测试中的出色稳定性。此外，与激光辅助转移法制备的碳膜相比，所获得的碳膜具有亲水性、低电阻性和多孔性，有利于能量存储设备的制造。为了证明其实际应用，我们在玻璃上制作了一个平面碳基微型超级电容器，该电容器表现出优异的电化学性能和循环性能。

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引用次数: 0

Elucidating silanol removal in MFI nanosized zeolites through controlled post-synthesis hydrothermal treatments 通过受控合成后水热处理阐明 MFI 纳米沸石中的硅醇去除作用

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105360

Hugo Cruchade, Francesco Dalena, Eddy Dib, Abdelhafid Aitblal, Diogenes Honorato Piva, Aymeric Magisson, Svetlana Mintova

The rational control of silanol groups is still an elusive dream in zeolite synthesis. To enhance our understanding of this phenomenon, we have performed various hydrothermal post-synthesis treatments on nanosized Silicalite-1 using sodium molybdate, sodium chloride, and ultrapure water to evaluate the alteration of silanol content. All treated samples exhibited a phase transition from orthorhombic to monoclinic confirmed by X-ray diffraction (XRD). Fourier-Transform Infrared (FTIR) and solid-state Nuclear Magnetic Resonance (NMR) spectroscopy showed a decrease in the concentration of silanol groups in the post treated samples. The treatment with sodium molybdate leads to the removal of approximately 98% of the silanol groups, while the samples treated with sodium chloride and ultrapure water showed a decrease of 90% and 20% respectively, compared to the parent silicalite-1. Additionally, the results from pyridine adsorption followed by FTIR show that the Parent-Silicalite-1 and the H₂O-Silicalite-1 samples contain a significant amount of defects, requiring 13.55 and 11.18 μmol, respectively, to saturate all the unsymmetrical bridging sites, while for the sample treated with sodium chloride only 1.07 µmol is needed to saturate all siloxane sites. In contrast, the treatment with sodium molybdate produced a free-defects zeolite. Molybdenum was found to contribute to the removal of both weak and strong hydrogen-bonded silanol groups through its insertion into the zeolite framework, while sodium played a significant role in condensing open bridges within the zeolite framework and removing less weak and strong hydrogen bonded silanol groups. This condensation of silanol groups seems to be facilitated by the polarization of silanol groups in presence of Na⁺ promoting the formation of siloxy groups that eventually condense easily with adjacent SiOH groups, liberating water molecules during the activation process of the samples.

合理控制硅醇基团仍然是沸石合成中一个难以实现的梦想。为了加深对这一现象的理解，我们使用钼酸钠、氯化钠和超纯水对纳米级 Silicalite-1 进行了各种水热合成后处理，以评估硅醇含量的变化。经 X 射线衍射 (XRD) 证实，所有处理过的样品都出现了从正方晶到单斜晶的相变。傅立叶变换红外光谱（FTIR）和固态核磁共振（NMR）光谱显示，后处理样品中硅醇基团的浓度有所下降。与母体硅灰石-1 相比，用钼酸钠处理可去除约 98% 的硅醇基团，而用氯化钠和超纯水处理的样品则分别减少了 90% 和 20%。此外，吡啶吸附后的傅立叶变换红外光谱结果表明，母体硅灰石-1 和 H2O 硅灰石-1 样品含有大量缺陷，分别需要 13.55 和 11.18 μmol 才能使所有非对称桥接位达到饱和，而用氯化钠处理的样品只需要 1.07 μmol 就能使所有硅氧烷位达到饱和。相比之下，用钼酸钠处理的沸石无缺陷。研究发现，钼通过插入沸石框架有助于去除弱和强氢键硅烷醇基团，而钠则在沸石框架内缩合开放桥和去除较弱和较强氢键硅烷醇基团方面发挥了重要作用。硅醇基团的缩合似乎是由于硅醇基团在 Na+ 存在下的极化促进了硅氧基团的形成，而硅氧基团最终很容易与相邻的 SiOH 基团缩合，在样品的活化过程中释放出水分子。

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引用次数: 0

Electrochemical corrosion behavior and passive film properties of Fe2Ni2CrV0.5Nbx (x=0.2, 0.4, 0.6, 0.8) eutectic high-entropy alloy coating prepared by laser cladding 激光熔覆制备的 Fe2Ni2CrV0.5Nbx (x=0.2, 0.4, 0.6, 0.8) 共晶高熵合金涂层的电化学腐蚀行为和被动膜特性

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105317

Hao Liu , Yingying Li , Peijian Chen , Xinhua Liu , Jingbin Hao , Haifeng Yang

The phase composition, microstructure morphology, and corrosion behavior of Fe₂Ni₂CrV_0.5Nb_x (x = 0.2, 0.4, 0.6, 0.8) eutectic high-entropy alloy (EHEA) coatings produced via laser cladding were investigated. The research delved into discerning the phase structures and microstructural variations of the EHEA coatings concerning differing Nb compositions. The findings highlighted a direct correlation between Nb content and the volume fraction of the eutectic structure, specifically the FCC/Laves phases. Electrochemical evaluations, including diverse tests such as potentiodynamic polarization, electrochemical impedance spectroscopy, cyclic polarization, Mott-Schottky measurements, and X-ray photoelectron spectroscopy, revealed distinct corrosion behaviors among the EHEA variants. Notably, the Fe₂Ni₂CrV_0.5Nb_0.2 coating exhibited relatively superior corrosion resistance compared with Fe₂Ni₂CrV_0.5Nb_x (x = 0.4,0.6,0.8) coatings, attributed to its lower corrosion current density (I_corr) and the formation of a thicker passive film with prolonged passivation duration. Conversely, the Fe₂Ni₂CrV_0.5Nb_0.8 coating, characterized by increased eutectic structures and grain boundary density, yielded a thicker yet non-uniform passive film with higher vacancy defects. This comprehensive exploration into the corrosion behavior and passive film properties of these EHEA coatings provides a reference for designing materials that hold promising implications for future corrosion-resistant material development in industrial parts repair applications.

研究了通过激光熔覆生产的 Fe2Ni2CrV0.5Nbx（x = 0.2、0.4、0.6、0.8）共晶高熵合金（EHEA）涂层的相组成、微观结构形态和腐蚀行为。研究深入探讨了不同铌成分的 EHEA 涂层的相结构和微观结构变化。研究结果表明，铌含量与共晶结构（特别是 FCC/Laves 相）的体积分数直接相关。电化学评估包括各种测试，如电位动力极化、电化学阻抗光谱、循环极化、Mott-Schottky 测量和 X 射线光电子能谱，这些评估揭示了不同 EHEA 变体之间截然不同的腐蚀行为。值得注意的是，与 Fe2Ni2CrV0.5Nbx（x = 0.4、0.6、0.8）涂层相比，Fe2Ni2CrV0.5Nb0.2 涂层表现出相对较强的耐腐蚀性，这归因于其较低的腐蚀电流密度（Icorr）和较厚的被动膜的形成以及较长的钝化持续时间。相反，Fe2Ni2CrV0.5Nb0.8 涂层的特点是共晶结构和晶界密度增加，形成的被动膜较厚但不均匀，空位缺陷较多。对这些 EHEA 涂层的腐蚀行为和被动膜特性的全面探索为设计材料提供了参考，对未来工业零部件维修应用中的耐腐蚀材料开发具有重要意义。

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引用次数: 0

Optimizing the resistivity of colloidal SnO2 thin films by ion implantation and annealing 通过离子注入和退火优化二氧化锡胶体薄膜的电阻率

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105325

Abubakar Sadiq Yusuf , Martin Markwitz , Zhan Chen , Maziar Ramezani , John V. Kennedy , Holger Fiedler

Tin oxide (SnO₂) is a critical material for a wide range of applications, such as in perovskite solar cells, gas sensors, as well as for photocatalysis. For these applications the transparency to visible light, high availability, cheap fabrication process and high conductivity of SnO₂ benefits its commercial deployment. In this paper, we demonstrate that the resistivity of widely colloidal SnO₂ can be reduced by noble gas ion beam modification. After low energy argon implantation with a fluence of 4×10¹⁵ at.cm⁻² at 25keV and annealing at 200°C in air, the resistivity of as-deposited film was reduced from (178±6)μΩcm to (133±5)μΩcm, a reduction of 25%. Hall effect measurements showed that the primary cause of this is the increase in carrier concentration from (8.1±0.3)×10²⁰ cm⁻³ to (9.9±0.3)×10²⁰ cm⁻³. Annealing at 200°C resulted in the removal of defect clusters introduced by implantation, while annealing at 300°C resulted in the oxidation of the films, increasing their resistivity. The concentration of oxygen vacancy defects can be controlled by a combination of low energy noble gas ion implantation and annealing, providing promising performance increases for potential applications of SnO₂ where a low resistivity is crucial.

氧化锡（SnO2）是一种应用广泛的关键材料，如用于过氧化物太阳能电池、气体传感器以及光催化。在这些应用中，二氧化锡对可见光的透明性、高可用性、廉价的制造工艺和高导电性都有利于其商业应用。在本文中，我们证明了通过惰性气体离子束改性可以降低广泛胶体二氧化锡的电阻率。在 25keV 下以 4×1015 at.cm-2 的通量进行低能氩离子注入并在 200°C 的空气中退火后，沉积薄膜的电阻率从 (178±6)μΩcm 降低到 (133±5)μΩcm，降低了 25%。霍尔效应测量结果表明，主要原因是载流子浓度从 (8.1±0.3)×1020 cm-3 增加到 (9.9±0.3)×1020 cm-3。200°C 退火可去除植入过程中引入的缺陷簇，而 300°C 退火则会导致薄膜氧化，增加其电阻率。氧空位缺陷的浓度可通过低能惰性气体离子植入和退火相结合的方法加以控制，从而有望提高对电阻率要求较低的二氧化锡的潜在应用性能。

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引用次数: 0

Tailoring the morphology of poly (triazine imide) by chemical equilibrium towards enhanced photocatalytic overall water splitting 通过化学平衡调整聚（三嗪亚胺）的形态以增强光催化整体水分离能力

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-28 DOI: 10.1016/j.surfin.2024.105321

Jiawen Yu , Jun Zhang , Qin Wang, Wenjie Zhou, Mengdie Cai, Jia-qi Bai, Qin Cheng, Jingshuai Chen, Song Sun

Poly (triazine imide) generally obtained via ionothermal synthesis typically exhibits nanosheet or hexagonal prism aggregation. This study presents an innovative approach to modulate PTI morphology without the addition of structure-directing agents. By manipulating the volatilization rate of gaseous substances like ammonia, various PTI morphologies were achieved. The results indicate that adjusting chemical equilibrium conditions favors the formation of morphologies with higher surface energy, leading to increased specific surface area and morphological variations. Notably, these changes do not alter the crystal structure, elemental composition or band gap, but significantly impact the dynamics of photogenerated carriers. Additionally, this morphological transformation not only increase the surface active sites but also enhance the interfacial interaction between the cocatalyst and the PTI support. Among the morphologies, rod-like PTI exhibit superior photocatalytic performance, with hydrogen evolution and oxygen evolution of 506.8 μmol h^-1 g^-1 and of 234.0 μmol h^-1 g^-1, respectively, representing a 15.8-fold increase over the original sample. Furthermore, the manipulation of chemical equilibrium during polymerization offers new insights and potential for advancing crystalline carbon nitride-based photocatalyst.

通过离子热合成法获得的聚三嗪酰亚胺通常呈纳米片状或六方棱柱状聚集。本研究提出了一种无需添加结构引导剂即可调节 PTI 形态的创新方法。通过操纵氨等气态物质的挥发率，实现了各种 PTI 形态。结果表明，调整化学平衡条件有利于形成表面能更高的形态，从而增加比表面积和形态变化。值得注意的是，这些变化不会改变晶体结构、元素组成或带隙，但会对光生载流子的动力学产生重大影响。此外，这种形态变化不仅增加了表面活性位点，还增强了催化剂与 PTI 支持物之间的界面相互作用。在这些形态中，棒状 PTI 表现出更优越的光催化性能，氢进化和氧进化分别达到 506.8 μmol h-1 g-1 和 234.0 μmol h-1 g-1，比原始样品提高了 15.8 倍。此外，在聚合过程中操纵化学平衡为推进基于氮化碳的结晶光催化剂的发展提供了新的见解和潜力。

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引用次数: 0

Experimental study and molecular dynamics simulation of Ag/Ti diffusion bonding 银/钛扩散键的实验研究与分子动力学模拟

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-26 DOI: 10.1016/j.surfin.2024.105296

Liuyong Wang , Hao Wang , Qingyi Zou , Yue Li , Min Lei , Wenqin Wang , Yulong Li

The diffusion kinetics and mechanisms of Ag/Ti diffusion couple were investigated through experiments and molecular dynamics simulations. The influence of processing parameters, such as temperature (700 °C to 850 °C) and holding time (15 min to 60 min), on microstructure and phase formation at the Ag/Ti joint was studied. In addition, the mechanical properties of the joints were evaluated. IMCs including AgTi, Ti₂Ag, and the Ti(ss, Ag) solid solution exist at the diffusion interface. The activation energy for the growth of the TiAg phase is 98 kJ/mol. Molecular dynamics simulations show that Ag has a higher diffusion coefficient (5.0×10^-5 m²/s) compared to Ti (2.5×10^-8 m²/s). Meanwhile, the grains at the TiAg/Ti interface are significantly smaller than those at the TiAg/Ag side. These results indicate that the diffusion flux of Ag is higher than that of Ti, and the TiAg phase priority is formed at the interface. The grain boundary diffusion is a diffusion control mechanism. The Ti(ss, Ag) solid solution at the interface exhibits the highest nano-hardness and modulus, with values of 4.2 ± 0.1 GPa and 139.6 ± 0.6 GPa, respectively. The joint brazed at 750 °C for 30 min shows a maximum shear strength of 98 MPa, with fractures primarily occurring at the interface between the Ag and TiAg phases. This study provides insights into the diffusion behavior, phase formation dynamics, and mechanical properties of Ag/Ti diffusion couples, offering implications for the development of advanced materials in various engineering applications.

通过实验和分子动力学模拟研究了 Ag/Ti 扩散耦合的扩散动力学和机制。研究了温度（700 °C 至 850 °C）和保温时间（15 分钟至 60 分钟）等加工参数对 Ag/Ti 接头微观结构和相形成的影响。此外，还评估了接头的机械性能。扩散界面上存在包括 AgTi、Ti2Ag 和 Ti（ss，Ag）固溶体在内的 IMC。TiAg 相生长的活化能为 98 kJ/mol。分子动力学模拟显示，与 Ti（2.5×10-8 m2/s）相比，Ag 的扩散系数更高（5.0×10-5 m2/s）。同时，TiAg/Ti 界面的晶粒明显小于 TiAg/Ag 侧的晶粒。这些结果表明，Ag 的扩散通量高于 Ti 的扩散通量，在界面上形成了 TiAg 相优先。晶界扩散是一种扩散控制机制。界面上的 Ti（ss，Ag）固溶体表现出最高的纳米硬度和模量，分别为 4.2 ± 0.1 GPa 和 139.6 ± 0.6 GPa。在 750 °C 下钎焊 30 分钟的接头显示出 98 兆帕的最大剪切强度，断裂主要发生在 Ag 相和 TiAg 相之间的界面上。这项研究深入揭示了银/钛扩散偶的扩散行为、相形成动力学和力学性能，为各种工程应用中先进材料的开发提供了启示。

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引用次数: 0

Novel synergistic mechanism of oxalic acid -CMC at the solid-liquid interface: For selective depression of talc from chalcopyrite 草酸-CMC 在固液界面上的新型协同机制：从黄铜矿中选择性去除滑石

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-25 DOI: 10.1016/j.surfin.2024.105345

Hulin Gao , Jian Liu , Jiamei Hao , Xu Bai , Runpeng Liao

Flotation separation of chalcopyrite and talc is challenging due to their surface hydrophobicity, requiring a selective depressant for talc to achieve high-quality copper concentrate. This study is the first to use oxalic acid (OA) and carboxymethyl cellulose (CMC) as combined depressants for talc, and investigated the depression mechanism through flotation tests and various analysis techniques. Mixed minerals-flotation results showed that with 60+60 mg/L OA+CMC, talc was strongly depressed (10.16% recovery) with slight chalcopyrite (86.54% recovery) impact. The selective depression effect of OA+CMC was further verified through actual ore flotation experiments. Contact angle and zeta potential test indicated that OA+CMC significantly increased the hydrophobicity difference between talc and chalcopyrite surfaces. Adsorption capacity and atomic force microscope(AFM) results further confirmed that OA promotes CMC adsorption on talc surface, forming a dense CMC layer, whereas CMC adsorption on chalcopyrite was relatively low. Scanning electron microscope energy spectrum spectroscopy (SEM-EDS), fourier transform infrared spectroscopy(FTIR), and molecular dynamics (MD) results indicate that the synergistic depression mechanism of OA and CMC involves the formation of multiple adsorption layers at the solid-liquid interface, leading to an increased presence of hydrophilic groups on the talc surface, which results in its depression.

由于黄铜矿和滑石的表面疏水性，它们的浮选分离具有挑战性，需要一种对滑石有选择性的抑制剂，以获得高质量的铜精矿。本研究首次使用草酸（OA）和羧甲基纤维素（CMC）作为滑石的联合抑制剂，并通过浮选试验和各种分析技术研究了抑制机制。混合矿物浮选结果表明，在 60+60 mg/L OA+CMC 的条件下，滑石受到强烈抑制（回收率为 10.16%），黄铜矿受到轻微影响（回收率为 86.54%）。实际矿石浮选实验进一步验证了 OA+CMC 的选择性抑制效果。接触角和 Zeta 电位测试表明，OA+CMC 显著增加了滑石和黄铜矿表面的疏水性差异。吸附容量和原子力显微镜（AFM）结果进一步证实，OA 能促进 CMC 在滑石表面的吸附，形成致密的 CMC 层，而 CMC 在黄铜矿上的吸附量相对较低。扫描电子显微镜能谱（SEM-EDS）、傅立叶变换红外光谱（FTIR）和分子动力学（MD）结果表明，OA 和 CMC 的协同抑制机制包括在固液界面形成多个吸附层，导致滑石表面亲水基团的增加，从而导致其抑制作用。

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引用次数: 0

Surface modification and patterning of polymer thin films by plasma and adsorption behavior of proteins 等离子体对聚合物薄膜的表面改性和图案化以及蛋白质的吸附行为

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-25 DOI: 10.1016/j.surfin.2024.105342

Athul Nakulan , K. Sumithra , S. Sheethal , S. Yuvaraj , P. Peranantham , Y.L. Jeyachandran

The surface wettability property of hydrophobic polystyrene (PS) and hydrophilic polyethylene glycol (PEG) thin films subjected to modification by direct current plasma glow discharge is studied. The polymer films exhibited change of surface wettability on exposure to air, nitrogen, oxygen or argon plasmas. In PS films a swift modification to hydrophilic surface and subsequent steady recovery following first order kinetics are observed. The rate of modification and recovery are adjustable by adjusting the plasma ambient and parameters, and additional wet-chemical treatment using ionic solutions. In PEG films the hydrophobic wettability evolve with ageing following the first order kinetics, and is stable for long period on exposure to air ambient. Moreover, a vapor deposition like process is possible using the PEG films as source to deposit self-assembled molecular layers with hydrophobic wettability on other surfaces. Using surface modification or molecular deposition processes, the fabrication of wettability patterns in the surface of PS and PEG films, and on other surfaces by vapor transport using PEG films, and also the possibility to produce gradient wettability patterns are demonstrated. Moreover, the adsorption behavior of immuno-specific system of proteins on surface modified hydrophilic PS films is studied.

研究了通过直流等离子体辉光放电改性疏水性聚苯乙烯（PS）和亲水性聚乙二醇（PEG）薄膜的表面润湿性能。聚合物薄膜在暴露于空气、氮气、氧气或氩气等离子体时，表面润湿性发生了变化。在聚苯乙烯薄膜中，可以观察到亲水性表面迅速发生改性，随后按照一阶动力学稳定恢复。通过调整等离子环境和参数以及使用离子溶液进行额外的湿化学处理，可以调节改性和恢复的速度。在 PEG 薄膜中，疏水润湿性会随着老化按照一阶动力学发生变化，并且在暴露于空气环境中长期保持稳定。此外，还可以利用 PEG 薄膜作为源，在其他表面沉积具有疏水润湿性的自组装分子层，从而实现类似气相沉积的工艺。利用表面改性或分子沉积工艺，可以在 PS 和 PEG 薄膜表面形成润湿性图案，也可以通过 PEG 薄膜的气相传输在其他表面形成润湿性图案，还可以形成梯度润湿性图案。此外，还研究了免疫特异性蛋白质系统在表面改性亲水 PS 薄膜上的吸附行为。

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引用次数: 0

Constructing a Z-scheme heterojunction of oxygen-deficient WO3-x and g-C3N4 for superior photocatalytic evolution of H2 构建缺氧 WO3-x 和 g-C3N4 的 Z 型异质结，实现卓越的 H2 光催化进化能力

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-25 DOI: 10.1016/j.surfin.2024.105346

Fengyun Su, Mengzhen Tian, Hailong Cao, Zhishuai Wang, Qiang Zhao, Haiquan Xie, Yezhen Zhang, Xiaoli Jin, Xin Li, Zhengdao Li

Semiconductor-based photocatalytic water splitting enables the conversion of abundant solar energy to green and renewable hydrogen energy. Graphitic carbon nitride (g-C₃N₄) is synthesized using a straightforward method, demonstrating stable physicochemical properties and possessing an optimal bandgap, thus positioning it as a promising photocatalyst in the realm of environmental sustainability. Oxygen vacancies are extensively employed to modulate light absorption and surface properties of metal-oxide semiconductors. In this study, g-C₃N₄ nanosheets were coupled with oxygen-deficient tungsten trioxide (WO_3-x) to form heterojunction photocatalysts (X-WOCN). Comprehensive material characterization results demonstrated that the constructed heterojunction extended the visible light absorption range, improved photogenerated electron-hole separation efficiency, and thus augmented photocatalytic activity. Notably, the optimum hydrogen evolution rate of 6 %-WOCN was enhanced by 5.4-fold compared to that of g-C₃N₄. Furthermore, we propose a Z-scheme heterojunction charge separation mechanism mediated by oxygen defects and support this mechanism through detection of surface-active substances •O₂⁻ and •OH. This study offers novel propositions into the function of oxygen defects in facilitating charge separation within Z-scheme heterojunction.

基于半导体的光催化水分离技术可将丰富的太阳能转化为绿色可再生氢能。氮化石墨碳（g-C3N4）是用一种简单的方法合成的，具有稳定的物理化学特性和最佳带隙，因此在环境可持续发展领域是一种很有前途的光催化剂。氧空位被广泛用于调节金属氧化物半导体的光吸收和表面特性。在这项研究中，g-C3N4 纳米片与缺氧的三氧化钨（WO3-x）结合形成了异质结光催化剂（X-WOCN）。综合材料表征结果表明，所构建的异质结扩大了可见光吸收范围，提高了光生电子-空穴分离效率，从而增强了光催化活性。值得注意的是，与 g-C3N4 相比，6%-WOCN 的最佳氢进化率提高了 5.4 倍。此外，我们还提出了一种由氧缺陷介导的 Z 型异质结电荷分离机制，并通过检测表面活性物质 -O2- 和 -OH 支持了这一机制。这项研究为氧缺陷在促进 Z 型异质结电荷分离方面的功能提供了新的命题。

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引用次数: 0

Plasma assisted single-step synthesis of carbon-coated SrFe2O4 electrodes for enhancing supercapacitor and oxygen evolution reaction 等离子体辅助单步合成碳涂层 SrFe2O4 电极，用于增强超级电容器和氧进化反应

IF 5.7 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Surfaces and Interfaces

Pub Date : 2024-10-24 DOI: 10.1016/j.surfin.2024.105339

Kumaresan Lakshmanan , Amarnath Pasupathi , Bharani Narayanan , Yugeswaran Subramaniam , Shanmugavelayutham Gurusamy

Developing highly efficient, conductive, and porous electrode materials for superior electrochemical bifunctional applications presents a formidable challenge, particularly when considering impurity-free large-scale production. This investigation focuses on synthesizing a composite material of highly conductive amorphous carbon-coated SrFe₂O₄ nanoparticles to enhance supercapacitor and oxygen evolution performance. The C@SrFe₂O₄ nanoparticles were synthesized through a thermal plasma process utilizing argon, methane, and carbon dioxide gas environments. The prepared samples' phase, crystal structure, morphology, elemental composition, and chemical state analysis were thoroughly examined. The electrochemical performance of the prepared samples, including Fe₃O₄, SrO, and C@SrFe₂O₄ electrodes, was evaluated for their suitability in electrochemical capacitor applications. Remarkably, C@SrFe₂O₄ nanoparticles exhibited notable electrochemical pseudocapacitive behavior, demonstrating a significantly higher specific capacitance of 588.7 F/g at a current density of 1 A/g. Moreover, at a current density of 10 A/g, the C@SrFe₂O₄ electrode exhibited outstanding cycling stability, maintaining 91 % of its initial capacitance over 5000 charge-discharge cycles. Furthermore, it showcased exceptional and uniform electrocatalytic activity for the OER, requiring only 186 mV in overpotentials to achieve a current density of 10 mA/ cm². These findings underscore the potential of mesoporous C@SrFe₂O₄ nanoparticles as promising materials for supercapacitors and OER applications.

为卓越的电化学双功能应用开发高效、导电和多孔电极材料是一项艰巨的挑战，尤其是在考虑无杂质大规模生产的情况下。本研究的重点是合成一种高导电性无定形碳包覆 SrFe2O4 纳米粒子的复合材料，以提高超级电容器和氧气进化的性能。C@SrFe2O4 纳米粒子是利用氩气、甲烷和二氧化碳气体环境，通过热等离子体工艺合成的。对所制备样品的相貌、晶体结构、形态、元素组成和化学态分析进行了深入研究。对所制备样品（包括 Fe3O4、SrO 和 C@SrFe2O4 电极）的电化学性能进行了评估，以确定其在电化学电容器应用中的适用性。值得注意的是，C@SrFe2O4 纳米粒子表现出显著的电化学伪电容行为，在电流密度为 1 A/g 时，比电容高达 588.7 F/g。此外，在 10 A/g 的电流密度下，C@SrFe2O4 电极表现出卓越的循环稳定性，在 5000 次充放电循环中保持了 91% 的初始电容。此外，它还显示出卓越而均匀的 OER 电催化活性，只需要 186 mV 的过电位就能达到 10 mA/ cm2 的电流密度。这些发现强调了介孔 C@SrFe2O4 纳米粒子作为超级电容器和 OER 应用材料的潜力。

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