Pub Date : 2024-11-05DOI: 10.1016/j.surfin.2024.105306
Wentao Luo , Xing Wei , Jiaxin Wang , Yan Zhang , Yun Yang , Jian Liu , Ye Tian , Li Duan
In the face of the urgent need for energy transition, Z-scheme heterojunctions are considered highly suitable candidates for future photocatalytic applications, owing to their exceptional optoelectronic characteristics and high catalytic efficiency. This paper systematically investigates the geometric structure, optoelectronic properties, and catalytic efficiency of the GeSe/PtS2 heterojunction through detailed first-principles calculations. The findings indicate that the band structure of the GeSe/PtS2 heterojunction presents a staggered Type-Ⅱ band alignment and exhibits an indirect band gap measuring 1.75 eV Charge transfer analysis reveals that under the interplay of an intrinsic electric field directed from GeSe to PtS2 and the band bending occurring at the heterojunction interface, the GeSe/PtS2 heterojunction conforms to the obvious Z-scheme electron transfer mechanism characteristics. This facilitates the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) to proceed smoothly on opposite sides of the heterojunction. Across the pH range of 0 to 14, the heterojunction's band edge positions successfully span the redox potentials of water, and can still meet the hydrolysis potential requirements under strain. In addition, the GeSe/PtS2 heterojunction not only effectively compensates for the poor absorption of PtS2 monolayer to visible light, but also achieves a wider visible light absorption range through the strain-induced redshift in the spectrum. At the same time, the solar to hydrogen (STH) efficiency of up to 15.56 % further underscores the substantial catalytic potential of the GeSe/PtS2 heterojunction, offering promising design strategies for a technological revolution in the field of photocatalysis.
{"title":"Theoretical design of Z-scheme photocatalyst for water splitting with excellent catalytic performance: GeSe/PtS2 heterojunction","authors":"Wentao Luo , Xing Wei , Jiaxin Wang , Yan Zhang , Yun Yang , Jian Liu , Ye Tian , Li Duan","doi":"10.1016/j.surfin.2024.105306","DOIUrl":"10.1016/j.surfin.2024.105306","url":null,"abstract":"<div><div>In the face of the urgent need for energy transition, Z-scheme heterojunctions are considered highly suitable candidates for future photocatalytic applications, owing to their exceptional optoelectronic characteristics and high catalytic efficiency. This paper systematically investigates the geometric structure, optoelectronic properties, and catalytic efficiency of the GeSe/PtS<sub>2</sub> heterojunction through detailed first-principles calculations. The findings indicate that the band structure of the GeSe/PtS<sub>2</sub> heterojunction presents a staggered Type-Ⅱ band alignment and exhibits an indirect band gap measuring 1.75 eV Charge transfer analysis reveals that under the interplay of an intrinsic electric field directed from GeSe to PtS<sub>2</sub> and the band bending occurring at the heterojunction interface, the GeSe/PtS<sub>2</sub> heterojunction conforms to the obvious Z-scheme electron transfer mechanism characteristics. This facilitates the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) to proceed smoothly on opposite sides of the heterojunction. Across the pH range of 0 to 14, the heterojunction's band edge positions successfully span the redox potentials of water, and can still meet the hydrolysis potential requirements under strain. In addition, the GeSe/PtS<sub>2</sub> heterojunction not only effectively compensates for the poor absorption of PtS<sub>2</sub> monolayer to visible light, but also achieves a wider visible light absorption range through the strain-induced redshift in the spectrum. At the same time, the solar to hydrogen (STH) efficiency of up to 15.56 % further underscores the substantial catalytic potential of the GeSe/PtS<sub>2</sub> heterojunction, offering promising design strategies for a technological revolution in the field of photocatalysis.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105306"},"PeriodicalIF":5.7,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660615","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1016/j.surfin.2024.105369
Yang Yu , Yang An , Ran Chen , Shihang Rao , Dingyuan Tang , Yajun Deng , Qingxia Liu
Natural gas hydrates are non-stoichiometric crystalline compounds composed of natural gas and water, typically found in the pore spaces constructed by minerals. Mineral crystals exhibit significant variations in surface properties among different crystal facets. Despite the importance of these mineral crystal facets, previous studies have not reported their influence on natural gas hydrates. To address this gap, we focused on quartz, a vital component of hydrate reservoirs, and studied the process of natural gas hydrates formation and dissociation on its distinct crystal facets. In our investigation, we simplified pores as narrow gap spaces between two parallel quartz substrates, and captured the entire process with a microscope. The results indicate that the formation and dissociation of natural gas hydrates are notably influenced by the distinct crystal facets of quartz. The influences of quartz crystal facet on the hydrate formation are primarily attributed to two factors, wettability and hydroxyl concentration of quartz crystal facet. We have also revealed the mechanism of how quartz crystal facet influences the hydrate dissociation. This research provides a fundamental understanding of how mineral crystal facets influence the hydrate formation and dissociation, offering a novel perspective for the design of processes for extracting hydrate.
{"title":"Effects of crystal facets of quartz on the formation and dissociation of natural gas hydrates","authors":"Yang Yu , Yang An , Ran Chen , Shihang Rao , Dingyuan Tang , Yajun Deng , Qingxia Liu","doi":"10.1016/j.surfin.2024.105369","DOIUrl":"10.1016/j.surfin.2024.105369","url":null,"abstract":"<div><div>Natural gas hydrates are non-stoichiometric crystalline compounds composed of natural gas and water, typically found in the pore spaces constructed by minerals. Mineral crystals exhibit significant variations in surface properties among different crystal facets. Despite the importance of these mineral crystal facets, previous studies have not reported their influence on natural gas hydrates. To address this gap, we focused on quartz, a vital component of hydrate reservoirs, and studied the process of natural gas hydrates formation and dissociation on its distinct crystal facets. In our investigation, we simplified pores as narrow gap spaces between two parallel quartz substrates, and captured the entire process with a microscope. The results indicate that the formation and dissociation of natural gas hydrates are notably influenced by the distinct crystal facets of quartz. The influences of quartz crystal facet on the hydrate formation are primarily attributed to two factors, wettability and hydroxyl concentration of quartz crystal facet. We have also revealed the mechanism of how quartz crystal facet influences the hydrate dissociation. This research provides a fundamental understanding of how mineral crystal facets influence the hydrate formation and dissociation, offering a novel perspective for the design of processes for extracting hydrate.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105369"},"PeriodicalIF":5.7,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142661079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1016/j.surfin.2024.105356
Xuzhao Han , Yue Xing , Hailin Zhang , Dongbin Zhang , Lan Hao , Zhenbing Xie , Yuwei Wang
Prussian blue analogues (PBAs) are promising energy storage materials for supercapacitors. However, high defects and low activity are challenging for high-performance of PBAs. Herein, we propose a series of modified copper Prussian blue analogues (CFPs) with interface rearrangement followed by F modification and Na enrichment. The spectroscopic and electrochemical characteristics demonstrated the synergistic effect of F and Na, revealing the advantages of efficient electronic control and reaction sites synergism, which contributes to the high ion/electron transport and reversibility of CFPs. Benefitting from the reduced defects, optimized conductivity, and boosted electrochemically active surface and exposed active sites resulting from pre-stored Na and regulated F, the supercapacitor performance of CFP-3 has been improved, with a specific capacity of 182 F g−1 at 1 A g−1, and the rate capability is 82.4 % of the initial specific capacitance at 10 A g−1, which is 4 times higher than that of unmodified CFP-0. Asymmetric CFP-3//CNT device achieves an energy density of 6.1 Wh kg−1 at a power density of 1 kW kg−1, and an energy density of 5.3 Wh kg−1 at a power density of 7 kW kg−1. After 10,000 cycles, the device still retains 82.4 %, showing good cyclic stability. This work proposes a new approach to improve the energy storage properties by rearranging the interfacial atomic and optimizing the electrochemically active sites, which provides a new guidance for designing high-performance supercapacitor materials.
普鲁士蓝类似物(PBAs)是很有前途的超级电容器储能材料。然而,高缺陷和低活性是高性能普鲁士蓝类似物面临的挑战。在此,我们提出了一系列经过界面重排、F修饰和Na富集修饰的铜普鲁士蓝类似物(CFPs)。光谱和电化学特性显示了 F 和 Na 的协同效应,揭示了高效电子控制和反应位点协同的优势,这有助于 CFPs 的高离子/电子传输和可逆性。得益于预存储 Na 和调控 F 所带来的缺陷减少、电导率优化、电化学活性表面和暴露活性位点增强,CFP-3 的超级电容器性能得到了改善,在 1 A g-1 时的比容量为 182 F g-1,在 10 A g-1 时的速率能力为初始比电容的 82.4%,是未改性 CFP-0 的 4 倍。非对称 CFP-3/CNT 器件在功率密度为 1 kW kg-1 时的能量密度为 6.1 Wh kg-1,在功率密度为 7 kW kg-1 时的能量密度为 5.3 Wh kg-1。经过 10,000 次循环后,该装置仍能保持 82.4 % 的能量密度,显示出良好的循环稳定性。这项工作提出了一种通过重新排列界面原子和优化电化学活性位点来提高储能性能的新方法,为设计高性能超级电容器材料提供了新的指导。
{"title":"Synergistic effect of Na enrichment and F modification on copper Prussian blue analogue nanoparticles for supercapacitors","authors":"Xuzhao Han , Yue Xing , Hailin Zhang , Dongbin Zhang , Lan Hao , Zhenbing Xie , Yuwei Wang","doi":"10.1016/j.surfin.2024.105356","DOIUrl":"10.1016/j.surfin.2024.105356","url":null,"abstract":"<div><div>Prussian blue analogues (PBAs) are promising energy storage materials for supercapacitors. However, high defects and low activity are challenging for high-performance of PBAs. Herein, we propose a series of modified copper Prussian blue analogues (CFPs) with interface rearrangement followed by F modification and Na enrichment. The spectroscopic and electrochemical characteristics demonstrated the synergistic effect of F and Na, revealing the advantages of efficient electronic control and reaction sites synergism, which contributes to the high ion/electron transport and reversibility of CFPs. Benefitting from the reduced defects, optimized conductivity, and boosted electrochemically active surface and exposed active sites resulting from pre-stored Na and regulated F, the supercapacitor performance of CFP-3 has been improved, with a specific capacity of 182 F <em>g</em><sup>−1</sup> at 1 A <em>g</em><sup>−1</sup>, and the rate capability is 82.4 % of the initial specific capacitance at 10 A <em>g</em><sup>−1</sup>, which is 4 times higher than that of unmodified CFP-0. Asymmetric CFP-3//CNT device achieves an energy density of 6.1 Wh kg<sup>−1</sup> at a power density of 1 kW kg<sup>−1</sup>, and an energy density of 5.3 Wh kg<sup>−1</sup> at a power density of 7 kW kg<sup>−1</sup>. After 10,000 cycles, the device still retains 82.4 %, showing good cyclic stability. This work proposes a new approach to improve the energy storage properties by rearranging the interfacial atomic and optimizing the electrochemically active sites, which provides a new guidance for designing high-performance supercapacitor materials.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105356"},"PeriodicalIF":5.7,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142661081","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-04DOI: 10.1016/j.surfin.2024.105396
Moutaz Aldrdery , Muhammad Aadil , Awais Khalid , Mazen R. Alrahili , Muawya Elhadi , Faisal Alresheedi , Meri Algarni , Mohamed.R. El-Aassar , Atef El Jery
Herein, novel hierarchical Gd@WO3 pom-pom-like microstructures have been prepared through the hydrothermal method and combined with RGO sheets (denoted as RGO/Gd@WO3). The synthesized materials, along with their analogs, were characterized through X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), Fourier transform infrared (FT-IR), Mott-Schottky, current-voltage (I-V), electrochemical impedance spectroscopy (EIS), and optical analyses. The unique morphology of pom-pom-like microstructures allowed better interaction with pollutant molecules. Rare earth element (Gd3+) ions act as trapping species for photo-generated electrons and prolong the life span of reactive oxygen species (ROS). The high conductivity and flexible nature of RGO sheets provided fast transport of active species and provided stability to the photocatalytic material. To test the photocatalytic efficiency of RGO/Gd@WO3, crystal violet (CV) and acetylsalicylic acid (ASA) were used as model pollutants. Under a mimetic light source, RGO/Gd@WO3 exhibited maximum photodegradation of 98.8 % and 84 % for CV and ASA within 120 min of irradiation, respectively. Photocurrent, Mott-Schottky, and EIS experiments proved the production, effective separation, and transmission of photo-active species in the presence of RGO/Gd@WO3 as compared to Gd@WO3 and WO3. Given the electrochemical testing and optical analysis, the photocatalytic mechanism is anticipated for the high photocatalytic activity of RGO/Gd@WO3. The novel RGO/Gd@WO3 photocatalyst proved to be a superior photocatalytic material for the photodegradation of organic pollutants.
{"title":"Hydrothermally synthesized hierarchical Pom-Pom-like gadolinium modified tungsten oxide reinforced with rGO for annihilation of acetylsalicylic acid and crystal violet","authors":"Moutaz Aldrdery , Muhammad Aadil , Awais Khalid , Mazen R. Alrahili , Muawya Elhadi , Faisal Alresheedi , Meri Algarni , Mohamed.R. El-Aassar , Atef El Jery","doi":"10.1016/j.surfin.2024.105396","DOIUrl":"10.1016/j.surfin.2024.105396","url":null,"abstract":"<div><div>Herein, novel hierarchical Gd@WO<sub>3</sub> pom-pom-like microstructures have been prepared through the hydrothermal method and combined with RGO sheets (denoted as RGO/Gd@WO<sub>3</sub>). The synthesized materials, along with their analogs, were characterized through X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), Fourier transform infrared (FT-IR), Mott-Schottky, current-voltage (I-V), electrochemical impedance spectroscopy (EIS), and optical analyses. The unique morphology of pom-pom-like microstructures allowed better interaction with pollutant molecules. Rare earth element (Gd<sup>3+</sup>) ions act as trapping species for photo-generated electrons and prolong the life span of reactive oxygen species (ROS). The high conductivity and flexible nature of RGO sheets provided fast transport of active species and provided stability to the photocatalytic material. To test the photocatalytic efficiency of RGO/Gd@WO<sub>3</sub>, crystal violet (CV) and acetylsalicylic acid (ASA) were used as model pollutants. Under a mimetic light source, RGO/Gd@WO<sub>3</sub> exhibited maximum photodegradation of 98.8 % and 84 % for CV and ASA within 120 min of irradiation, respectively. Photocurrent, Mott-Schottky, and EIS experiments proved the production, effective separation, and transmission of photo-active species in the presence of RGO/Gd@WO<sub>3</sub> as compared to Gd@WO<sub>3</sub> and WO<sub>3</sub>. Given the electrochemical testing and optical analysis, the photocatalytic mechanism is anticipated for the high photocatalytic activity of RGO/Gd@WO<sub>3</sub>. The novel RGO/Gd@WO<sub>3</sub> photocatalyst proved to be a superior photocatalytic material for the photodegradation of organic pollutants.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105396"},"PeriodicalIF":5.7,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660719","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-04DOI: 10.1016/j.surfin.2024.105395
Yanlong Yu , Yuan Tao , Sai Yan
In this investigation, we explored two series of composites comprising p-type α-MnS with selectively exposed {001} or {111} facets, coated with n-type ZIF-67 nanoparticles, to enhance the photocatalytic activity on Rhodamine B (RhB) degradation. The influence of the crystal facet orientation and the p-n junction on the photocatalytic efficacy was also well studied. The α-MnS/ZIF-67 composites displayed enhanced separation of charge carriers and superior light absorption capabilities, benefiting for efficient photocatalysis. The composites with cubic α-MnS morphology exhibited a pronouncedly higher photocatalytic activity relative to those with octahedral α-MnS morphology. The composition of α-MnS with ZIF-67 constructed the formation of a p-n junction with build-in electric field, extending the response into the visible region and promoting the mobility of charge carriers, thereby improving the photocatalytic performance. Our findings revealed that superoxide radicals (O2-) were the major reactive species in the photocatalytic degradation process. This study contributes novel insights into the development of high-performance and stable metal-organic framework (MOF)-based photocatalysts through the crystal facet engineering and the construction of p-n junctions.
在这项研究中,我们探索了两种系列的复合材料,它们由具有选择性暴露的{001}或{111}面的 p 型 α-MnS 组成,表面包覆有 n 型 ZIF-67 纳米粒子,以增强对罗丹明 B(RhB)降解的光催化活性。研究还深入探讨了晶面取向和 p-n 结对光催化效率的影响。α-MnS/ZIF-67复合材料显示出更强的电荷载体分离能力和卓越的光吸收能力,有利于高效光催化。与八面体 α-MnS 形状的复合材料相比,立方体 α-MnS 形状的复合材料具有更高的光催化活性。α-MnS与ZIF-67的组合构建了一个具有内置电场的p-n结,将响应扩展到可见光区域,促进了电荷载流子的迁移,从而提高了光催化性能。我们的研究结果表明,超氧自由基(O2-)是光催化降解过程中的主要反应物。这项研究为通过晶面工程和构建 p-n 结来开发高性能、稳定的金属有机框架(MOF)光催化剂提供了新的见解。
{"title":"Efficient photocatalytic activity over α-MnS/ZIF-67 p-n junction: Revealing the synergistic effects of exposed crystal facets and built-in electric field mechanism","authors":"Yanlong Yu , Yuan Tao , Sai Yan","doi":"10.1016/j.surfin.2024.105395","DOIUrl":"10.1016/j.surfin.2024.105395","url":null,"abstract":"<div><div>In this investigation, we explored two series of composites comprising p-type α-MnS with selectively exposed {001} or {111} facets, coated with n-type ZIF-67 nanoparticles, to enhance the photocatalytic activity on Rhodamine B (RhB) degradation. The influence of the crystal facet orientation and the p-n junction on the photocatalytic efficacy was also well studied. The α-MnS/ZIF-67 composites displayed enhanced separation of charge carriers and superior light absorption capabilities, benefiting for efficient photocatalysis. The composites with cubic α-MnS morphology exhibited a pronouncedly higher photocatalytic activity relative to those with octahedral α-MnS morphology. The composition of α-MnS with ZIF-67 constructed the formation of a p-n junction with build-in electric field, extending the response into the visible region and promoting the mobility of charge carriers, thereby improving the photocatalytic performance. Our findings revealed that superoxide radicals (O<sub>2</sub><sup>-</sup>) were the major reactive species in the photocatalytic degradation process. This study contributes novel insights into the development of high-performance and stable metal-organic framework (MOF)-based photocatalysts through the crystal facet engineering and the construction of p-n junctions.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105395"},"PeriodicalIF":5.7,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142661084","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-04DOI: 10.1016/j.surfin.2024.105377
Amit Sahu, Céline Dupont
In spite of the growing interest in maghemite, its structure is not accurately known, and numerous uncertainties remain. The ongoing debate centers on its crystalline structure, whether cubic or tetragonal, and its implications for stable surface terminations. This study explores the crystalline nature of maghemite — cubic versus tetragonal — and its effects on surface stability. Using density functional theory (DFT) with Hubbard corrections, we evaluated the stability and electronic properties of maghemite’s (001) and (111) surfaces under both cubic and tetragonal configurations, while also considering the influence of a Pt substrate and strain arising from lattice mismatch. Our findings indicate that native cubic (001) surfaces are inherently more stable than tetragonal ones. However, the presence of a Pt substrate shifts this stability, favoring the cubic (111) surface presenting a higher adhesion energy. We examined the electronic properties of various cases to provide a rationalization of the observed stability order. Our study provides crucial insights into the impact of crystalline structure and Pt substrate on the stability and favored terminations of maghemite surfaces, emphasizing their prospective utility as water oxidation catalysts.
{"title":"Maghemite surface termination variations: Influence of models and Pt substrate","authors":"Amit Sahu, Céline Dupont","doi":"10.1016/j.surfin.2024.105377","DOIUrl":"10.1016/j.surfin.2024.105377","url":null,"abstract":"<div><div>In spite of the growing interest in maghemite, its structure is not accurately known, and numerous uncertainties remain. The ongoing debate centers on its crystalline structure, whether cubic or tetragonal, and its implications for stable surface terminations. This study explores the crystalline nature of maghemite — cubic versus tetragonal — and its effects on surface stability. Using density functional theory (DFT) with Hubbard corrections, we evaluated the stability and electronic properties of maghemite’s (001) and (111) surfaces under both cubic and tetragonal configurations, while also considering the influence of a Pt substrate and strain arising from lattice mismatch. Our findings indicate that native cubic (001) surfaces are inherently more stable than tetragonal ones. However, the presence of a Pt substrate shifts this stability, favoring the cubic (111) surface presenting a higher adhesion energy. We examined the electronic properties of various cases to provide a rationalization of the observed stability order. Our study provides crucial insights into the impact of crystalline structure and Pt substrate on the stability and favored terminations of maghemite surfaces, emphasizing their prospective utility as water oxidation catalysts.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105377"},"PeriodicalIF":5.7,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594133","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The copper (Cu)/tantalum (Ta) nanofilms are the vital component in the through silicon via (TSV) wafer. However, the current lack of research on the ultra-precision machining of Cu/Ta nanofilms limits the development of TSV-based 3D integration technologies. In this work, molecular dynamics simulations are conducted to reveal the microstructure and interface evolution mechanism of Cu/Ta nanofilms during nano-grinding under various grinding depths. The results show that the material removal mode differs between the Cu and Ta layers, and the thickness of the subsurface damage layer of the Cu layer is greater than that of the Ta layer. The Cu/Ta interface is well stabilized, and small amounts of micro-defects appear only at larger grinding depths after grinding. The lattice mismatch of the constituent layers and the hindering role by the interface lead to stress concentration at the interface, and it is more obvious with increasing grinding depth. Nevertheless, there is a significant stress release after grinding. Our computations indicate that the competition between the evolution of interfacial structures and discrepancies in the physical properties of constituent layers leads to an increase in grinding forces at the interface. Furthermore, the heat transfer is obstructed by the Cu/Ta interface. This study provides valuable insights into the grinding mechanisms of Cu/Ta nanofilms, which is conducive to further improving the manufacturing process of the TSV wafer and enhancing the performance of microelectronic devices.
铜(Cu)/钽(Ta)纳米薄膜是硅通孔(TSV)晶片的重要组成部分。然而,由于目前缺乏对铜/钽纳米薄膜超精密加工的研究,限制了基于 TSV 的三维集成技术的发展。本研究通过分子动力学模拟揭示了不同研磨深度下纳米研磨过程中铜/钽纳米薄膜的微观结构和界面演化机理。结果表明,Cu 层和 Ta 层的材料去除模式不同,且 Cu 层的表面下损伤层厚度大于 Ta 层。Cu/Ta 界面稳定良好,磨削后只有在较大的磨削深度才会出现少量微缺陷。组成层的晶格失配和界面的阻碍作用导致了界面处的应力集中,并且随着研磨深度的增加应力集中现象更加明显。尽管如此,磨削后仍有明显的应力释放。我们的计算表明,界面结构的演变与组成层物理性质的差异之间的竞争导致了界面研磨力的增加。此外,Cu/Ta 界面阻碍了热传递。这项研究为了解 Cu/Ta 纳米薄膜的研磨机制提供了宝贵的见解,有利于进一步改进 TSV 硅片的制造工艺,提高微电子器件的性能。
{"title":"Atomic-scale insights into the microstructure and interface evolution mechanism of copper/tantalum nanofilms during ultra-precision grinding","authors":"Kezhong Xu, Yuqi Zhou, Yuhan Gao, Yuxin Chen, Xin Lei, Ziniu Yu, Fulong Zhu","doi":"10.1016/j.surfin.2024.105393","DOIUrl":"10.1016/j.surfin.2024.105393","url":null,"abstract":"<div><div>The copper (Cu)/tantalum (Ta) nanofilms are the vital component in the through silicon via (TSV) wafer. However, the current lack of research on the ultra-precision machining of Cu/Ta nanofilms limits the development of TSV-based 3D integration technologies. In this work, molecular dynamics simulations are conducted to reveal the microstructure and interface evolution mechanism of Cu/Ta nanofilms during nano-grinding under various grinding depths. The results show that the material removal mode differs between the Cu and Ta layers, and the thickness of the subsurface damage layer of the Cu layer is greater than that of the Ta layer. The Cu/Ta interface is well stabilized, and small amounts of micro-defects appear only at larger grinding depths after grinding. The lattice mismatch of the constituent layers and the hindering role by the interface lead to stress concentration at the interface, and it is more obvious with increasing grinding depth. Nevertheless, there is a significant stress release after grinding. Our computations indicate that the competition between the evolution of interfacial structures and discrepancies in the physical properties of constituent layers leads to an increase in grinding forces at the interface. Furthermore, the heat transfer is obstructed by the Cu/Ta interface. This study provides valuable insights into the grinding mechanisms of Cu/Ta nanofilms, which is conducive to further improving the manufacturing process of the TSV wafer and enhancing the performance of microelectronic devices.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105393"},"PeriodicalIF":5.7,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660716","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-03DOI: 10.1016/j.surfin.2024.105391
Lailla Daianna Soltau Missio Pinheiro , Gabriela Geraldo Sangoi , Nicole Camponogara Righi , Bruno Stefanello Vizzotto , Yolice Patricia Moreno Ruiz , André Galembeck , Giovani Pavoski , Denise Crocce Romano Espinosa , Alencar Kolinski Machado , William Leonardo da Silva
The present work aims to synthesize, characterize, and evaluate the cytotoxicity and antimicrobial activity of PLA/PCL polymeric nanocomposite with silver nanoparticles (AgNPs) and copper (CuNPs) and the addition of lavender essential oil (LEO) for application in tissue engineering. For the synthesis of the nanocomposite films, the central composite rotational design (CCRD 2²) was used, where the ideal condition was 0 .5 %wt. of AgNPs and CuNPs (3:1D) with a higher cell viability (196.1 %) after 24 h. After defining the ideal condition, the effect of incorporating LEO into the polymer blend and nanoparticles in the proportions of 0.5 (3:1D0.5), 0.75 (3:1D0.75) and 1 v-1 (3:1D1) was evaluated. All nanocomposite films were characterized structurally, morphologically, thermally, and mechanically by X-ray diffraction (XRD), Field Emission Gun–Scanning Electron Microscopy (FEG-SEM), Thermogravimetric analysis (TGA), contact angle and mechanical Properties (displacement and maximum tension). To evaluate cytotoxicity, an in vitro safety profile was performed in HFF-1 (fibroblasts) and HaCat (keratinocytes) cell lines, where PLA/PCL polymer blend with 0.5 %wt. of AgNPs and CuNPs (3:1D) and PLA/PCL polymer blend with 0.5 %wt. of AgNPs and CuNPs and LEO (0.5 v-1) (3:1D0.5) nanocomposite film showed the best cell viability without the nitric oxide (NO) generation, total levels of reactive oxygen species (ROS) or dsDNA release for the HFF-1 and HaCat cell lines, as well as genoprotective characteristic and without genotoxic profile. Moreover, the tests were carried out on the pH of injured skin at different immersion times (3, 6, 12 and 24 h) and didn´t show cell death or inflammatory reaction. For the antimicrobial activity, the 3:1D, 3:1D0.5, and PLA/PCL polymer blend with 0.5 %wt. of AgNPs and CuNPs and LEO (0.75 v-1) (3:1D0.75) nanocomposite films showed the formation of biofilm for S. aureus, E. coli, P. aeruginosa and K. pneumoniae. Therefore, the PLA/PCL polymer nanocomposite with AgNPs and CuNPs showed potential application as a healing dressing for skin regeneration.
{"title":"PLA/PCL polymer nanocomposite with silver and copper nanoparticles and lavender essential oil: Synthesis, characterization and application in tissue engineering","authors":"Lailla Daianna Soltau Missio Pinheiro , Gabriela Geraldo Sangoi , Nicole Camponogara Righi , Bruno Stefanello Vizzotto , Yolice Patricia Moreno Ruiz , André Galembeck , Giovani Pavoski , Denise Crocce Romano Espinosa , Alencar Kolinski Machado , William Leonardo da Silva","doi":"10.1016/j.surfin.2024.105391","DOIUrl":"10.1016/j.surfin.2024.105391","url":null,"abstract":"<div><div>The present work aims to synthesize, characterize, and evaluate the cytotoxicity and antimicrobial activity of PLA/PCL polymeric nanocomposite with silver nanoparticles (AgNPs) and copper (CuNPs) and the addition of lavender essential oil (LEO) for application in tissue engineering. For the synthesis of the nanocomposite films, the central composite rotational design (CCRD 2²) was used, where the ideal condition was 0 .5 %wt. of AgNPs and CuNPs (3:1D) with a higher cell viability (196.1 %) after 24 h. After defining the ideal condition, the effect of incorporating LEO into the polymer blend and nanoparticles in the proportions of 0.5 (3:1D0.5), 0.75 (3:1D0.75) and 1 v<sup>-1</sup> (3:1D1) was evaluated. All nanocomposite films were characterized structurally, morphologically, thermally, and mechanically by X-ray diffraction (XRD), Field Emission Gun–Scanning Electron Microscopy (FEG-SEM), Thermogravimetric analysis (TGA), contact angle and mechanical Properties (displacement and maximum tension). To evaluate cytotoxicity, an <em>in vitro</em> safety profile was performed in HFF-1 (fibroblasts) and HaCat (keratinocytes) cell lines, where PLA/PCL polymer blend with 0.5 %wt. of AgNPs and CuNPs (3:1D) and PLA/PCL polymer blend with 0.5 %wt. of AgNPs and CuNPs and LEO (0.5 v<sup>-1</sup>) (3:1D0.5) nanocomposite film showed the best cell viability without the nitric oxide (NO) generation, total levels of reactive oxygen species (ROS) or dsDNA release for the HFF-1 and HaCat cell lines, as well as genoprotective characteristic and without genotoxic profile. Moreover, the tests were carried out on the pH of injured skin at different immersion times (3, 6, 12 and 24 h) and didn´t show cell death or inflammatory reaction. For the antimicrobial activity, the 3:1D, 3:1D0.5, and PLA/PCL polymer blend with 0.5 %wt. of AgNPs and CuNPs and LEO (0.75 v<sup>-1</sup>) (3:1D0.75) nanocomposite films showed the formation of biofilm for <em>S. aureus, E. coli, P. aeruginosa</em> and <em>K. pneumoniae</em>. Therefore, the PLA/PCL polymer nanocomposite with AgNPs and CuNPs showed potential application as a healing dressing for skin regeneration.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105391"},"PeriodicalIF":5.7,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142661085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-03DOI: 10.1016/j.surfin.2024.105390
Felipe Barría-Cáceres , Felipe A. Angel
Aiming at the formation of graded junctions, specifically the utilization of perovskite-perovskite homojunctions, we have successfully developed a reproducible methodology for synthesizing perovskite films using dual deposition of organic and inorganic precursors through vacuum thermal evaporation, forming compositionally modulated FAPbI3-based perovskite materials. These homojunctions leverage the self-compositional doping of perovskite materials, incorporating both n-doped and p-doped films. We employed complementary techniques such as energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), and glow discharge optical emission spectroscopy (GDOES) to characterize these films. The combination of our deposition technique and comprehensive spectroscopic analysis provides valuable insights into the composition and properties of the resulting films. By employing this novel methodology, we aim to advance the development of new processing methods for the synthesis of compositionally doped perovskite films and paving the way for their potential applications to fabricate solar cells that include perovskite-perovskite homojunctions, enhancing charge extraction at the interface.
为了形成分级结,特别是利用透辉石-透辉石同质结,我们成功地开发了一种可重复的方法,通过真空热蒸发,利用有机和无机前驱体的双重沉积合成透辉石薄膜,形成成分调制的基于 FAPbI3 的透辉石材料。这些同质结充分利用了透辉石材料的自成分掺杂特性,同时结合了 n 掺杂和 p 掺杂薄膜。我们采用了能量色散 X 射线光谱 (EDS)、X 射线光电子能谱 (XPS) 和辉光放电光学发射光谱 (GDOES) 等补充技术来表征这些薄膜。我们的沉积技术与全面的光谱分析相结合,为了解薄膜的组成和特性提供了宝贵的信息。通过采用这种新颖的方法,我们旨在推动合成成分掺杂的包晶石薄膜的新加工方法的发展,并为其在太阳能电池制造中的潜在应用铺平道路,这些太阳能电池包括包晶石-包晶石同结,从而增强了界面上的电荷提取。
{"title":"Validation of spectroscopy quantitative method for the synthesis of compositionally-modulated FAPbI3 perovskite films by thermal evaporation","authors":"Felipe Barría-Cáceres , Felipe A. Angel","doi":"10.1016/j.surfin.2024.105390","DOIUrl":"10.1016/j.surfin.2024.105390","url":null,"abstract":"<div><div>Aiming at the formation of graded junctions, specifically the utilization of perovskite-perovskite homojunctions, we have successfully developed a reproducible methodology for synthesizing perovskite films using dual deposition of organic and inorganic precursors through vacuum thermal evaporation, forming compositionally modulated FAPbI<sub>3</sub>-based perovskite materials. These homojunctions leverage the self-compositional doping of perovskite materials, incorporating both n-doped and p-doped films. We employed complementary techniques such as energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), and glow discharge optical emission spectroscopy (GDOES) to characterize these films. The combination of our deposition technique and comprehensive spectroscopic analysis provides valuable insights into the composition and properties of the resulting films. By employing this novel methodology, we aim to advance the development of new processing methods for the synthesis of compositionally doped perovskite films and paving the way for their potential applications to fabricate solar cells that include perovskite-perovskite homojunctions, enhancing charge extraction at the interface.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105390"},"PeriodicalIF":5.7,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142593843","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Salvianolic acid B (Sal B), the key bioactive compound in the traditional Chinese herb Salvia miltiorrhiza, is recognized for its extensive pharmacological effects, especially its potent cardioprotective properties. Network pharmacology analysis has elucidated the complex mechanisms of action of Sal B by integrating a systems biology framework with the examination of multiple drug targets. Despite the therapeutic potential of Sal B, its precise detection remains a technical challenge, mostly because of interference in the detection of coexisting structural analogs in leach liquor. The adoption of electrochemical technology offers a practical alternative that meets the demands for speed and precision in quantifying Sal B. Consequently, the current study presents an electrochemical sensing approach based on the composite material Au@CeO2-Fe3O4 embellished reduced graphene oxide (rGO). This integration utilized the exceptional electrical conductivity of Au, the catalytic properties of ceria, and the magnetic properties of iron oxide (Fe3O4) nanoparticles, which significantly enhanced the sensor performance. The results indicate that the developed electrochemical sensor exhibited a linear detection range spanning four orders of magnitude, with a low detection limit of 0.037 μM. The linear range is 1–1000 μM, and the sensitivity is 59.44 µA µM⁻¹ cm⁻², demonstrating high sensitivity and selectivity in the detection of Sal B in actual samples. This research provides a novel perspective for the efficient detection of Sal B, offering a scientific basis for clinical therapeutic monitoring and contributing positively to the modernization of traditional Chinese medicine.
丹酚酸 B(Sal B)是传统中草药丹参中的主要生物活性化合物,因其广泛的药理作用,尤其是强效的心脏保护特性而得到公认。通过将系统生物学框架与多个药物靶点的研究相结合,网络药理学分析阐明了 Sal B 的复杂作用机制。尽管 Sal B 具有治疗潜力,但其精确检测仍然是一项技术挑战,主要原因是浸出液中共存结构类似物的检测存在干扰。因此,本研究提出了一种基于 Au@CeO2-Fe3O4 缀合还原氧化石墨烯(rGO)复合材料的电化学传感方法。这种集成利用了金的优异导电性、铈的催化特性和氧化铁(Fe3O4)纳米颗粒的磁性,从而显著提高了传感器的性能。结果表明,所开发的电化学传感器的线性检测范围跨越了四个数量级,检测限低至 0.037 μM。其线性范围为 1-1000 μM,灵敏度为 59.44 µA µM-¹ cm-²,显示了在实际样品中检测盐 B 的高灵敏度和高选择性。该研究为高效检测盐酸乙胺提供了新的视角,为临床治疗监测提供了科学依据,为中药现代化做出了积极贡献。
{"title":"Analysis of the highly sensitive mechanism of an electrochemical sensor for salvianolic acid B based on network pharmacology","authors":"Zihua Wang, Yue Han, Weiru Tan, Pengshuai Zhang, Lulu Guo, Jing Tian, Shuoye Yang, Lu Zhang","doi":"10.1016/j.surfin.2024.105388","DOIUrl":"10.1016/j.surfin.2024.105388","url":null,"abstract":"<div><div>Salvianolic acid B (Sal B), the key bioactive compound in the traditional Chinese herb <em>Salvia miltiorrhiza</em>, is recognized for its extensive pharmacological effects, especially its potent cardioprotective properties. Network pharmacology analysis has elucidated the complex mechanisms of action of Sal B by integrating a systems biology framework with the examination of multiple drug targets. Despite the therapeutic potential of Sal B, its precise detection remains a technical challenge, mostly because of interference in the detection of coexisting structural analogs in leach liquor. The adoption of electrochemical technology offers a practical alternative that meets the demands for speed and precision in quantifying Sal B. Consequently, the current study presents an electrochemical sensing approach based on the composite material Au@CeO<sub>2</sub>-Fe<sub>3</sub>O<sub>4</sub> embellished reduced graphene oxide (rGO). This integration utilized the exceptional electrical conductivity of Au, the catalytic properties of ceria, and the magnetic properties of iron oxide (Fe<sub>3</sub>O<sub>4</sub>) nanoparticles, which significantly enhanced the sensor performance. The results indicate that the developed electrochemical sensor exhibited a linear detection range spanning four orders of magnitude, with a low detection limit of 0.037 μM. The linear range is 1–1000 μM, and the sensitivity is 59.44 µA µM⁻¹ cm⁻², demonstrating high sensitivity and selectivity in the detection of Sal B in actual samples. This research provides a novel perspective for the efficient detection of Sal B, offering a scientific basis for clinical therapeutic monitoring and contributing positively to the modernization of traditional Chinese medicine.</div></div>","PeriodicalId":22081,"journal":{"name":"Surfaces and Interfaces","volume":"55 ","pages":"Article 105388"},"PeriodicalIF":5.7,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142660623","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}