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The essential synergy between experiments and theory in applied surface science 应用表面科学中实验与理论的重要协同作用
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-30 DOI: 10.1016/j.apsadv.2024.100651
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引用次数: 0
Manufacturing and properties characterization of Ti patterned coatings for water electrolyzers by CSAM 利用 CSAM 分析水电解槽钛花纹涂层的制造和性能特征
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-25 DOI: 10.1016/j.apsadv.2024.100649
This work investigates the microstructure and manufacturing control of the masked Cold Spray Additive Manufacturing (CSAM) strategy for producing of new bipolar plates (BPPs) for Proton Exchange Membrane (PEM) electrolyzers, using low-cost, lightweight, and machinable materials. CSAM is a solid-state process capable of fabricating 3D patterned parts based on a bottom-up approach using masks with a desired pattern. This study focuses on the dimensional and microstructural characteristics of pin fins fabricated with spherical (Ti-S) and irregular (Ti-I) Ti powders using the masked CSAM technology. Additionally, the performance of both Ti parts for its application in PEM electrolyzers was evaluated in terms of corrosion resistance and interfacial contact resistance (ICR). The results demonstrated that the masked CSAM technology allowed precise control and customization of the dimensions of the 3D-printed pin fins, obtaining porosity values of 6 ± 1 % for Ti-S and 4 ± 1 % for Ti-I. The evaluation of the corrosion resistance of the CSAM Ti patterned parts showed that for both Ti-S and Ti-I powders a stable oxide film at the typical operation potential (1.8 V vs Ag/AgCl) of a PEM water electrolyzer was formed without signs of pitting corrosion. Finally, at a compaction pressure of 150 N/cm2 ICR values of 42 ± 19, 40 ± 13, and 24 ± 7 mΩ·cm2 were obtained for Ti-I, Ti-S, and standard Ti Bulk, respectively. The results suggest than the masked CSAM technology shows great potential for the fabrication of Ti BPPs.
这项研究探讨了掩模冷喷增材制造(CSAM)战略的微观结构和制造控制,该战略用于使用低成本、轻质和可加工材料生产质子交换膜(PEM)电解器的新型双极板(BPP)。CSAM 是一种固态工艺,能够基于自下而上的方法,使用带有所需图案的掩模制造三维图案部件。本研究的重点是利用掩模 CSAM 技术,研究球形(Ti-S)和不规则(Ti-I)钛粉末制造的针翅片的尺寸和微观结构特征。此外,还从耐腐蚀性和界面接触电阻 (ICR) 的角度评估了这两种钛部件在 PEM 电解槽中的应用性能。结果表明,遮蔽式 CSAM 技术可以精确控制和定制 3D 打印针翅片的尺寸,Ti-S 的孔隙率值为 6 ± 1 %,Ti-I 的孔隙率值为 4 ± 1 %。对 CSAM Ti 图形部件耐腐蚀性的评估表明,Ti-S 和 Ti-I 粉末在 PEM 水电解槽的典型工作电位(1.8 V 对 Ag/AgCl)下形成了稳定的氧化膜,没有点蚀迹象。最后,在 150 N/cm2 的压实压力下,Ti-I、Ti-S 和标准 Ti Bulk 的 ICR 值分别为 42 ± 19、40 ± 13 和 24 ± 7 mΩ-cm2。这些结果表明,掩模 CSAM 技术在制造钛 BPP 方面具有巨大的潜力。
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引用次数: 0
Exploring the role of edges in surface functionalization and stability of plasma-modified carbon materials: Experimental and DFT insights 探索边缘在等离子体改性碳材料的表面功能化和稳定性中的作用:实验和 DFT 见解
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-23 DOI: 10.1016/j.apsadv.2024.100648
Effective surface functionalization of carbon nanomaterials plays a crucial role in various applications. We investigated the impact of edges on surface functionalization and stability of oxygen-modified carbon materials using a combination of experimental techniques and Density Functional Theory (DFT) insights. Graphenic paper, highly oriented pyrolytic graphite (HOPG), and graphenic flakes were employed as model systems, with oxygen plasma treatment (generator power 100 W, oxygen pressure 0.2 mbar, exposure time 6 – 300 s) serving as the modification method. Surface morphology and chemical composition were characterized using scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy. The results revealed the introduction of oxygen functional groups on the investigated carbon surfaces (up to 20 at % by XPS) whereas; the structural integrity of the materials remained intact upon plasma modification (SEM, Raman). Work function was used as a sensitive parameter for monitoring the surface changes (increase by ∼1.4 eV, 1.3 eV, and 1 eV for graphenic paper, HOPG, and graphenic flakes, respectively) while time-dependent measurements revealed distinct kinetic processes governing the decay of functionalization, highlighting the role of surface defects in post-plasma processes. DFT calculations provided molecular-level insights into the surface processes, elucidating the mechanisms underlying the diffusion of hydroxyls, their recombination, and water desorption. Since the calculated activation barrier for recombination on basal graphenic planes (∼1.0 eV) and edges (∼5.5 eV) are distinctly different, it can be thus concluded that the persistent functionalization is due to the surface edges. Our findings contribute to a deeper understanding of surface modification processes of carbon materials and offer rationales for the design of advanced functional nanomaterials with tailored surface properties.
碳纳米材料的有效表面功能化在各种应用中起着至关重要的作用。我们采用实验技术和密度泛函理论(DFT)相结合的方法,研究了边缘对氧改性碳材料表面官能化和稳定性的影响。以石墨烯纸、高取向热解石墨(HOPG)和石墨烯薄片为模型系统,采用氧等离子体处理(发生器功率 100 W,氧压 0.2 mbar,曝光时间 6 - 300 s)作为改性方法。使用扫描电子显微镜 (SEM)、X 射线光电子能谱 (XPS) 和拉曼光谱对其表面形貌和化学成分进行了表征。结果显示,所研究的碳表面引入了氧官能团(XPS 高达 20%),而等离子体改性后材料的结构完整性保持不变(扫描电镜、拉曼光谱)。功函数被用作监测表面变化的敏感参数(石墨烯纸、HOPG 和石墨烯薄片的功函数分别增加了 1.4 eV、1.3 eV 和 1 eV),而随时间变化的测量揭示了官能化衰减的独特动力学过程,突出了表面缺陷在等离子体后过程中的作用。DFT 计算为表面过程提供了分子层面的见解,阐明了羟基扩散、羟基重组和水脱附的基本机制。由于基底石墨烯平面(∼1.0 eV)和边缘(∼5.5 eV)上计算出的重组活化势垒截然不同,因此可以得出结论:持久官能化是由于表面边缘造成的。我们的发现有助于加深对碳材料表面改性过程的理解,并为设计具有定制表面特性的先进功能纳米材料提供了理论依据。
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引用次数: 0
Multidimensional woodchips-like Mn-metal-organic framework for asymmetric supercapacitor devices 用于不对称超级电容器设备的多维木片状锰金属有机框架
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-21 DOI: 10.1016/j.apsadv.2024.100650
Multidimensional manganese-metal organic frameworks (Mn-MOF) are synthesized using 1,2,4,5-Benzene tetracarboxylic acid (BTTC) at various temperatures (100–160 °C). The Fourier-transform infrared spectroscopy (FT-IR) and X-ray diffraction (XRD) techniques successfully confirm the formation of Mn-MOF. Among the various temperatures, the Mn-MOF synthesized at 140 °C (Mn-MOF@BTTC-140) is remarkable because it has excellent crystallinity and a unique morphology, i.e., woodchips-like structure. The synthesized Mn-MOF@BTTC materials are used in supercapacitor applications. In comparison to all materials, Mn-MOF@BTTC-140 revealed the maximum specific capacitance (Cs) of 627 F g-1 @ 1 A g-1, and it displayed 91 % capacitance retention even after the 6000 cycles at a current density of 10 A g-1. Furthermore, the supercapacitor device (SD) constructed using carbon nanofibers (CNF) as the negative electrode and Mn-MOF@BTTC-140 as the positive electrode delivered an energy density of 25 W h kg-1 at a power density of 532 W kg-1. Ultimately, LED lighting demonstrates that our fabricated materials suit practical applications.
使用 1,2,4,5-苯四甲酸(BTTC)在不同温度(100-160 °C)下合成了多维锰金属有机框架(Mn-MOF)。傅立叶变换红外光谱(FT-IR)和 X 射线衍射(XRD)技术成功证实了锰-MOF 的形成。在不同温度下合成的 Mn-MOF(Mn-MOF@BTTC-140)具有优异的结晶度和独特的形态,即类似木片的结构,因而引人注目。合成的 Mn-MOF@BTTC 材料可用于超级电容器。与所有材料相比,Mn-MOF@BTTC-140 的最大比电容(Cs)为 627 F g-1 @ 1 A g-1,即使在 10 A g-1 的电流密度下循环 6000 次,其电容保持率仍高达 91%。此外,以纳米碳纤维(CNF)为负极、Mn-MOF@BTTC-140 为正极构建的超级电容器装置(SD)在功率密度为 532 W kg-1 时,能量密度达到 25 W h kg-1。最终,LED 照明证明了我们制造的材料适合实际应用。
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引用次数: 0
Designing g-C3N4/NiFe2O4 S-scheme heterojunctions for efficient photocatalytic degradation of Rhodamine B and tetracycline hydrochloride 设计用于高效光催化降解罗丹明 B 和盐酸四环素的 g-C3N4/NiFe2O4 S 型异质结
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-20 DOI: 10.1016/j.apsadv.2024.100647
Semiconductor based photocatalysis is considered as an effective and sustainable approach for the efficient treatment of effluents containing organic dyes and pharmaceuticals. Herein, visible light responsive g-C3N4/ NiFe2O4 (CN/NF) composite photocatalysts were designed by sol-gel auto-combustion assisted calcination method using ethylene glycol (EG) as a chelating agent. Bidentate nature and lower molecular weight of EG favour slow hydrolysis of Ni2+ and Fe3+ ions followed by formation of homogenous gel phase which under auto-combustion produced NF precursors. Calcination of the mixture of dicyandiamide (DCDA) and predetermined amount of NF precursors at 550 °C for 4 h resulted in the formation of CN/NF nanocomposites in which NF nanoparticles are anchored on thick plates of porous CN. The construction of CN/NF S-scheme heterojunctions was established through XPS studies and scavenging tests. The 10CN/NF nanocomposite exhibited superior photocatalytic Rhodamine B (RhB) degradation efficiency (98.6 %) which is 2.7 and 3.1 folds superior than that of pure NF and CN respectively. Additionally, the photocatalytic performance of 10CN/NF for tetracycline hydrochloride (TCH) degradation was found to be 84.32 %. The degradation efficiency was around 1.75 and 2.6 times higher than that was observed for pristine NF and CN correspondingly. The current study will bring fresh insights into the synthesis of CN/NF heterojunctions with an S-scheme charge transfer channel for the efficient treatment of waste waters containing dyes and antibiotics.
基于半导体的光催化技术被认为是高效处理含有有机染料和药物的污水的一种有效且可持续的方法。本文以乙二醇(EG)为螯合剂,通过溶胶-凝胶自燃辅助煅烧法设计了可见光响应型 g-C3N4/ NiFe2O4 (CN/NF) 复合光催化剂。EG 的双螯合性质和较低的分子量有利于 Ni2+ 和 Fe3+ 离子的缓慢水解,随后形成均匀的凝胶相,在自燃烧条件下产生 NF 前体。在 550 °C 下煅烧双氰胺(DCDA)和预定量的 NF 前体混合物 4 小时后,形成了 CN/NF 纳米复合材料,其中 NF 纳米颗粒锚定在多孔 CN 的厚板上。通过 XPS 研究和清除测试,确定了 CN/NF S 型异质结的构建。10CN/NF 纳米复合材料表现出卓越的光催化罗丹明 B(RhB)降解效率(98.6%),分别是纯 NF 和 CN 的 2.7 倍和 3.1 倍。此外,10CN/NF 对盐酸四环素(TCH)降解的光催化性能为 84.32%。降解效率分别是原始 NF 和 CN 的 1.75 倍和 2.6 倍。目前的研究将为合成具有 S 型电荷转移通道的 CN/NF 异质结,从而高效处理含有染料和抗生素的废水带来新的启示。
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引用次数: 0
First-Principle Calculations of Interfacial Resistance between Nickel Silicide and Hyperdoped Silicon with N-Type Dopants Arsenic, Phosphorus, Antimony, Selenium and Tellurium 硅化镍与含有 N 型掺杂剂砷、磷、锑、硒和碲的高掺杂硅之间界面电阻的第一原理计算
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-12 DOI: 10.1016/j.apsadv.2024.100646
The interfacial resistance between NiSi2 and n-type doped Si was investigated using density functional theory calculations with hybrid functionals. We explored the resistance of Si at different doping concentrations by assigning an effective potential to each Si atom. Then, the valley filtering effect at the NiSi2/Si interface was estimated by comparing the transmission spectra of NiSi2 and Si. We also examined the interfacial resistance between NiSi2 and hyperdoped Si with substitutional n-type dopants, including pnictogen (P, As and Sb) and chalcogen (Se and Te) atoms. Two types of substitutional dopant structures (a single dopant and a dopant dimer) were considered. The formation and binding energies of a single P/Te and a P/Te dimer were investigated to understand the stability in Si. The resistances of Si with a single dopant and with a dopant dimer at high doping concentrations were calculated to show that the resistance as low as ∼ 4×1011Ω·cm2 can be achieved with a single dopant (P, As and Sb). However, at high doping concentration where a dopant dimer forms, a P dimer cannot effectively donate electrons, resulting in high resistance, while a Te dimer can still provide electrons, achieving a resistance of ∼ 2×1010Ω·cm2. Therefore, the chalcogen deep donor atoms (Se and Te) can be effective n-type donors and lower the silicide contact resistance at the interface where Si is extremely highly n-type doped.
我们使用混合函数的密度泛函理论计算研究了 NiSi2 和 n 型掺杂硅之间的界面电阻。我们为每个硅原子分配了一个有效电势,从而探索了不同掺杂浓度下的硅电阻。然后,通过比较 NiSi2 和 Si 的透射光谱,估算了 NiSi2/Si 界面的滤谷效应。我们还研究了 NiSi2 与超掺杂硅之间的界面电阻,其中包含取代 n 型掺杂剂,包括对掺杂原子(P、As 和 Sb)和掺杂原子(Se 和 Te)。研究考虑了两种置换掺杂结构(单一掺杂和掺杂二聚体)。研究了单一 P/Te 和 P/Te 二聚体的形成和结合能,以了解其在硅中的稳定性。计算了高掺杂浓度下含有单一掺杂剂和掺杂剂二聚体的硅的电阻,结果表明,单一掺杂剂(P、As 和 Sb)可实现低至 ∼ 4×10-11Ω-cm2 的电阻。然而,在高掺杂浓度下会形成掺杂二聚体,P 二聚体不能有效地提供电子,从而导致高电阻,而 Te 二聚体仍能提供电子,从而实现 ∼ 2×10-10Ω-cm2 的电阻。因此,在硅极度掺杂 n 型元素的界面上,查尔根深供体原子(Se 和 Te)可以成为有效的 n 型供体,并降低硅化物的接触电阻。
{"title":"First-Principle Calculations of Interfacial Resistance between Nickel Silicide and Hyperdoped Silicon with N-Type Dopants Arsenic, Phosphorus, Antimony, Selenium and Tellurium","authors":"","doi":"10.1016/j.apsadv.2024.100646","DOIUrl":"10.1016/j.apsadv.2024.100646","url":null,"abstract":"<div><div>The interfacial resistance between NiSi<sub>2</sub> and n-type doped Si was investigated using density functional theory calculations with hybrid functionals. We explored the resistance of Si at different doping concentrations by assigning an effective potential to each Si atom. Then, the valley filtering effect at the NiSi<sub>2</sub>/Si interface was estimated by comparing the transmission spectra of NiSi<sub>2</sub> and Si. We also examined the interfacial resistance between NiSi<sub>2</sub> and hyperdoped Si with substitutional n-type dopants, including pnictogen (P, As and Sb) and chalcogen (Se and Te) atoms. Two types of substitutional dopant structures (a single dopant and a dopant dimer) were considered. The formation and binding energies of a single P/Te and a P/Te dimer were investigated to understand the stability in Si. The resistances of Si with a single dopant and with a dopant dimer at high doping concentrations were calculated to show that the resistance as low as ∼ <span><math><mrow><mn>4</mn><mspace></mspace><mo>×</mo><msup><mrow><mn>10</mn></mrow><mrow><mo>−</mo><mn>11</mn></mrow></msup><mspace></mspace><mstyle><mi>Ω</mi></mstyle><mo>·</mo><mi>c</mi><msup><mrow><mi>m</mi></mrow><mn>2</mn></msup></mrow></math></span> can be achieved with a single dopant (P, As and Sb). However, at high doping concentration where a dopant dimer forms, a P dimer cannot effectively donate electrons, resulting in high resistance, while a Te dimer can still provide electrons, achieving a resistance of ∼ <span><math><mrow><mn>2</mn><mspace></mspace><mo>×</mo><msup><mrow><mn>10</mn></mrow><mrow><mo>−</mo><mn>10</mn></mrow></msup><mspace></mspace><mstyle><mi>Ω</mi></mstyle><mo>·</mo><mi>c</mi><msup><mrow><mi>m</mi></mrow><mn>2</mn></msup></mrow></math></span>. Therefore, the chalcogen deep donor atoms (Se and Te) can be effective n-type donors and lower the silicide contact resistance at the interface where Si is extremely highly n-type doped.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142418740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Strain-oxygen vacancies coupling in topotactic (La,Sr)Co3-δ thin films 拓扑结构(La,Sr)Co3-δ 薄膜中的应变-氧空位耦合
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-28 DOI: 10.1016/j.apsadv.2024.100644
Oxygen defect engineering is a widely used approach for tuning physical properties in oxides. Multivalent transition metal oxide La0.7Sr0.3CoO3-δ (LSCO) shows oxygen vacancy-driven metal-to-insulator transition (MIT) due to topotactic phase transition and its high oxygen vacancy tolerance. Here, we introduce strain as a new degree of freedom to study the strain-oxygen vacancy coupling effects and elucidate its impact on the electronic property in oxygen-deficient LSCO epitaxial thin films grown on SrTiO3 (100) single crystal. By combining the experimental results with density functional theory plus U (DFT+U) calculations, we reveal that 2.1 % in-plane tensile strain can stabilize the insulating state of LSCO with a surprisingly low concentration of oxygen vacancies, <0.5 %. This study reveals that the MIT in LSCO is governed by the combination of oxygen vacancies and strain, offering the potential for additional tuning knob of the material's electronic properties.
氧缺陷工程是调整氧化物物理性质的一种广泛应用的方法。多价过渡金属氧化物 La0.7Sr0.3CoO3-δ(LSCO)因其拓扑相变和对氧空位的高耐受性而显示出氧空位驱动的金属到绝缘体转变(MIT)。在此,我们引入应变作为新的自由度来研究应变-氧空位耦合效应,并阐明其对生长在 SrTiO3 (100) 单晶上的缺氧 LSCO 外延薄膜电子特性的影响。通过将实验结果与密度泛函理论加 U(DFT+U)计算相结合,我们发现 2.1 % 的面内拉伸应变可以稳定 LSCO 的绝缘状态,而氧空位的浓度却低得惊人,仅为 0.5 %。这项研究揭示了 LSCO 中的 MIT 受氧空位和应变的共同作用,为进一步调整材料的电子特性提供了可能性。
{"title":"Strain-oxygen vacancies coupling in topotactic (La,Sr)Co3-δ thin films","authors":"","doi":"10.1016/j.apsadv.2024.100644","DOIUrl":"10.1016/j.apsadv.2024.100644","url":null,"abstract":"<div><div>Oxygen defect engineering is a widely used approach for tuning physical properties in oxides. Multivalent transition metal oxide La<sub>0.7</sub>Sr<sub>0.3</sub>CoO<sub>3-δ</sub> (LSCO) shows oxygen vacancy-driven metal-to-insulator transition (MIT) due to topotactic phase transition and its high oxygen vacancy tolerance. Here, we introduce strain as a new degree of freedom to study the strain-oxygen vacancy coupling effects and elucidate its impact on the electronic property in oxygen-deficient LSCO epitaxial thin films grown on SrTiO<sub>3</sub> (100) single crystal. By combining the experimental results with density functional theory plus U (DFT+U) calculations, we reveal that 2.1 % <em>in-plane</em> tensile strain can stabilize the insulating state of LSCO with a surprisingly low concentration of oxygen vacancies, &lt;0.5 %. This study reveals that the MIT in LSCO is governed by the combination of oxygen vacancies and strain, offering the potential for additional tuning knob of the material's electronic properties.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142358740","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fluorine-free superhydrophobic surfaces by atmospheric pressure plasma deposition of silazane-based suspensions 通过常压等离子体沉积硅烷基悬浮液实现无氟超疏水性表面
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-27 DOI: 10.1016/j.apsadv.2024.100645
Atmospheric plasma is used to deposit superhydrophobic fluorine-free thin films onto a substrate. In this process, a suspension of micron size silica particles in a silazane based precursor is deposited in a single step using a dielectric barrier discharge plasma jet moving above the substrate. Thanks to an optimized configuration between the suspension injection and the plasma jet, the silazane precursor can be polymerized on the substrate surface but also, on silica particles to form additional micro size particles. The experimental parameters for optimal deposition are discussed, with emphasis on those leading to the formation of this dual roughness surface caused by the arrangement of both silica particles and particles generated from the precursor plasma polymerization. The combination of these two different length scales for the roughness leads to a decreased wettability of the coated substrate and a water contact angle larger than 150°.
大气等离子体用于在基底上沉积超疏水无氟薄膜。在这一工艺中,使用在基底上方移动的介质阻挡放电等离子体射流,将微米大小的二氧化硅颗粒悬浮在硅氮烷前体中,一步完成沉积。由于优化了悬浮液喷射和等离子体喷射之间的配置,硅烷前驱体不仅能在基底表面聚合,还能在二氧化硅颗粒上形成额外的微小颗粒。本文讨论了优化沉积的实验参数,重点是硅颗粒和前驱体等离子聚合产生的颗粒的排列所导致的双重粗糙表面的形成。这两种不同长度尺度的粗糙度结合在一起,导致涂层基底的润湿性降低,水接触角大于 150°。
{"title":"Fluorine-free superhydrophobic surfaces by atmospheric pressure plasma deposition of silazane-based suspensions","authors":"","doi":"10.1016/j.apsadv.2024.100645","DOIUrl":"10.1016/j.apsadv.2024.100645","url":null,"abstract":"<div><div>Atmospheric plasma is used to deposit superhydrophobic fluorine-free thin films onto a substrate. In this process, a suspension of micron size silica particles in a silazane based precursor is deposited in a single step using a dielectric barrier discharge plasma jet moving above the substrate. Thanks to an optimized configuration between the suspension injection and the plasma jet, the silazane precursor can be polymerized on the substrate surface but also, on silica particles to form additional micro size particles. The experimental parameters for optimal deposition are discussed, with emphasis on those leading to the formation of this dual roughness surface caused by the arrangement of both silica particles and particles generated from the precursor plasma polymerization. The combination of these two different length scales for the roughness leads to a decreased wettability of the coated substrate and a water contact angle larger than 150°.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142322329","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Current-voltage plots reveal details of the energy level alignment during photoelectron spectroscopy experiments 电流电压图揭示光电子能谱实验中能级排列的细节
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-24 DOI: 10.1016/j.apsadv.2024.100643
The photoelectron current Is emitted from samples exposed to soft X-rays, such as is the case during X-ray photoelectron spectroscopy (XPS) analyses, is dominated by secondary electrons (SE) with energies not exceeding several eVs. Because of that, both the magnitude and the direction of Is is highly sensitive to the applied sample bias Vs with the magnitude of just a few volts. By measuring current-voltage characteristics for a series of samples with different work functions ϕSA a clear correlation between ϕSA and the shape of the IsVs curves is demonstrated. While all IsVs plots have a characteristic “reversed S” shape, a clear and consistent shift towards positive Vs values is observed with increasing ϕSA. The effect is explained by variations in the contact potential Vc established between the sample and the spectrometer. For all samples there is an excellent agreement between the Vc values (derived by ultraviolet photoelectron spectroscopy from the SE cut-offs) and the critical Vs value at which the photocurrent begins to drop. Hence, simple to perform current-voltage measurements, provide a unique insight into the details of the energy level alignment between sample and the spectrometer. In particular, the sign and the magnitude of the contact potential as well as relative changes in the sample work function can be determined. The knowledge of these parameters is often essential for correct interpretation of XPS spectra.
暴露在软 X 射线下的样品(例如在 X 射线光电子能谱(XPS)分析过程中)发出的光电子电流 Is 主要由能量不超过几 eV 的次级电子(SE)构成。因此,Is 的大小和方向对施加的样品偏压 Vs 非常敏感,其大小仅为几伏。通过测量一系列具有不同工作函数 ϕSA 的样品的电流-电压特性,可以清楚地看出 ϕSA 与 Is-Vs 曲线形状之间的相关性。虽然所有的 Is-Vs 曲线图都具有 "反向 S "形状的特征,但随着 ϕSA 的增大,Vs 值明显一致地向正值偏移。样品和光谱仪之间建立的接触电势 Vc 的变化可以解释这种效应。对于所有样品,Vc 值(通过紫外光电子能谱从 SE 截断点得出)与光电流开始下降的临界 Vs 值之间非常一致。因此,通过简单的电流-电压测量,可以深入了解样品与光谱仪之间能级排列的细节。尤其是可以确定接触电势的符号和大小,以及样品功函数的相对变化。了解这些参数往往对正确解读 XPS 光谱至关重要。
{"title":"Current-voltage plots reveal details of the energy level alignment during photoelectron spectroscopy experiments","authors":"","doi":"10.1016/j.apsadv.2024.100643","DOIUrl":"10.1016/j.apsadv.2024.100643","url":null,"abstract":"<div><div>The photoelectron current <span><math><msub><mi>I</mi><mi>s</mi></msub></math></span> emitted from samples exposed to soft X-rays, such as is the case during X-ray photoelectron spectroscopy (XPS) analyses, is dominated by secondary electrons (SE) with energies not exceeding several eVs. Because of that, both the magnitude and the direction of <span><math><msub><mi>I</mi><mi>s</mi></msub></math></span> is highly sensitive to the applied sample bias <span><math><msub><mi>V</mi><mi>s</mi></msub></math></span> with the magnitude of just a few volts. By measuring current-voltage characteristics for a series of samples with different work functions <span><math><msub><mi>ϕ</mi><mrow><mi>S</mi><mi>A</mi></mrow></msub></math></span> a clear correlation between <span><math><msub><mi>ϕ</mi><mrow><mi>S</mi><mi>A</mi></mrow></msub></math></span> and the shape of the <span><math><mrow><msub><mi>I</mi><mi>s</mi></msub><mo>−</mo><msub><mi>V</mi><mi>s</mi></msub></mrow></math></span> curves is demonstrated. While all <span><math><mrow><msub><mi>I</mi><mi>s</mi></msub><mo>−</mo><msub><mi>V</mi><mi>s</mi></msub></mrow></math></span> plots have a characteristic “reversed S” shape, a clear and consistent shift towards positive <span><math><msub><mi>V</mi><mi>s</mi></msub></math></span> values is observed with increasing <span><math><msub><mi>ϕ</mi><mrow><mi>S</mi><mi>A</mi></mrow></msub></math></span>. The effect is explained by variations in the contact potential <span><math><msub><mi>V</mi><mi>c</mi></msub></math></span> established between the sample and the spectrometer. For all samples there is an excellent agreement between the <span><math><msub><mi>V</mi><mi>c</mi></msub></math></span> values (derived by ultraviolet photoelectron spectroscopy from the SE cut-offs) and the critical <span><math><msub><mi>V</mi><mi>s</mi></msub></math></span> value at which the photocurrent begins to drop. Hence, simple to perform current-voltage measurements, provide a unique insight into the details of the energy level alignment between sample and the spectrometer. In particular, the sign and the magnitude of the contact potential as well as relative changes in the sample work function can be determined. The knowledge of these parameters is often essential for correct interpretation of XPS spectra.</div></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666523924000710/pdfft?md5=e7539ecdd61a3d201d4b16c346018b53&pid=1-s2.0-S2666523924000710-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142314782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Investigation of mechanical morphological structural and electrochemical properties of PVD TiAlN coating: A detail experimental and its correlation with an analytical approach using the least square method 研究 PVD TiAlN 涂层的机械形态结构和电化学性能:详细实验及其与使用最小二乘法的分析方法的相关性
IF 7.5 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-20 DOI: 10.1016/j.apsadv.2024.100638

In this experimental investigation, a Physical Vapor Deposition (PVD) process was employed to deposit TiAlN coating onto a Si substrate. The nitrogen flow rate, bias voltage, and substrate-to-target distance were selected as input parameters, each with three different levels. The design of these input parameters was structured according to Taguchi's L9 Orthogonal Array (OA). Following deposition, the mechanical, microstructural, structural, and electrochemical properties of the TiAlN coating were meticulously characterized and analyzed to discern the influence of the selected parameters on its various properties. Microstructural analysis revealed a homogeneous structure throughout the film. Additionally, the mechanical properties of the film exhibited notable performance under the specified parameters. However, it was observed that no consistent trend could be identified across different properties concerning the applied parameters. To elucidate the complex relationships among these variables, the Least Squares Method (LSM) regression analysis technique was employed. This analytical approach facilitated the establishment of correlations among the diverse parameters, enhancing the understanding of their collective impact on the TiAlN coating properties. The understanding of analytical results will be useful for predicting the values between the two extremities to measure the performance parameters where the experimental results are not available.

在这项实验研究中,采用了物理气相沉积(PVD)工艺在硅基底上沉积 TiAlN 涂层。氮气流速、偏置电压和基底到目标的距离被选为输入参数,每个参数有三个不同的水平。这些输入参数的设计采用田口 L9 正交阵列(OA)结构。沉积后,对 TiAlN 涂层的机械、微观结构、结构和电化学特性进行了细致的表征和分析,以确定所选参数对其各种特性的影响。微观结构分析表明,整个薄膜具有均匀的结构。此外,在特定参数下,薄膜的机械性能也表现出显著的性能。然而,观察发现,在应用参数的不同特性之间并没有发现一致的趋势。为了阐明这些变量之间的复杂关系,我们采用了最小二乘法(LSM)回归分析技术。这种分析方法有助于建立不同参数之间的相关性,从而加深理解这些参数对 TiAlN 涂层性能的共同影响。对分析结果的理解将有助于预测两个极值之间的数值,从而在没有实验结果的情况下测量性能参数。
{"title":"Investigation of mechanical morphological structural and electrochemical properties of PVD TiAlN coating: A detail experimental and its correlation with an analytical approach using the least square method","authors":"","doi":"10.1016/j.apsadv.2024.100638","DOIUrl":"10.1016/j.apsadv.2024.100638","url":null,"abstract":"<div><p>In this experimental investigation, a Physical Vapor Deposition (PVD) process was employed to deposit TiAlN coating onto a Si substrate. The nitrogen flow rate, bias voltage, and substrate-to-target distance were selected as input parameters, each with three different levels. The design of these input parameters was structured according to Taguchi's L9 Orthogonal Array (OA). Following deposition, the mechanical, microstructural, structural, and electrochemical properties of the TiAlN coating were meticulously characterized and analyzed to discern the influence of the selected parameters on its various properties. Microstructural analysis revealed a homogeneous structure throughout the film. Additionally, the mechanical properties of the film exhibited notable performance under the specified parameters. However, it was observed that no consistent trend could be identified across different properties concerning the applied parameters. To elucidate the complex relationships among these variables, the Least Squares Method (LSM) regression analysis technique was employed. This analytical approach facilitated the establishment of correlations among the diverse parameters, enhancing the understanding of their collective impact on the TiAlN coating properties. The understanding of analytical results will be useful for predicting the values between the two extremities to measure the performance parameters where the experimental results are not available.</p></div>","PeriodicalId":34303,"journal":{"name":"Applied Surface Science Advances","volume":null,"pages":null},"PeriodicalIF":7.5,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666523924000667/pdfft?md5=a9cba5c63541262efe72510492925f2e&pid=1-s2.0-S2666523924000667-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142272104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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