Surface Science最新文献_第5页

Destruction of surface oxide on (100)W in high-temperature atomic carbon deposition

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-20 DOI: 10.1016/j.susc.2024.122689

E.V. Rut'kov, E.Y. Afanas'eva, N.R. Gall

引用次数: 0

Support-dependent modulation of Pt33 nanoparticles: Insights into oxygen interaction, stability, electronic properties, and geometric structure

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-20 DOI: 10.1016/j.susc.2024.122686

David S․ Rivera Rocabado , Michihisa Koyama

{"title":"Support-dependent modulation of Pt33 nanoparticles: Insights into oxygen interaction, stability, electronic properties, and geometric structure","authors":"David S․ Rivera Rocabado , Michihisa Koyama","doi":"10.1016/j.susc.2024.122686","DOIUrl":"10.1016/j.susc.2024.122686","url":null,"abstract":"<div><div>Understanding how support materials influence the properties of Pt nanoparticles is crucial for advancing catalyst development. Using density functional theory calculations, we examine the effects of graphene, MgO(100), α-Al<sub>2</sub>O<sub>3</sub>(0001), and SnO<sub>2</sub>(110) supports on O atom adsorption and the stability, electronic, and geometric properties of Pt<sub>33</sub> nanoparticles. Our findings reveal that all supports significantly enhance O atom adsorption at the Pt<sub>33</sub>/support interface, with varying implications for Pt atom detachment and nanoparticle stability. The strength of Pt–support interactions follows the order: graphene < MgO(100) < α-Al<sub>2</sub>O<sub>3</sub>(0001) < SnO<sub>2</sub>(110). Bond order analysis indicates that supports stabilize the Pt–Pt interactions in the supported Pt<sub>33</sub> and their outer shell atoms. Electronic equilibrium between Pt<sub>33</sub> and the support induces electron transfer from graphene, MgO(100), and α-Al<sub>2</sub>O<sub>3</sub>(0001) to Pt<sub>33</sub>, and from Pt<sub>33</sub> to SnO<sub>2</sub>(110), shifting the <em>d</em>-band center and influencing catalytic properties. Strain analysis reveals compressive and tensile effects on Pt–Pt distances, correlating with the Pt<sub>33</sub> adsorption energies and indicating a link between geometric changes and nanoparticle stability. These insights elucidate the role of supports in O atom adsorption mechanisms and the tuning of Pt nanoparticle properties, providing valuable guidance for designing advanced catalysts with enhanced efficiency and stability for applications in fuel cells, sensors, and environmental remediation.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"754 ","pages":"Article 122686"},"PeriodicalIF":2.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143150990","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chemical interaction and molecular growth of a highly dipolar merocyanine molecule on metal surfaces: A photoelectron spectroscopy study

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-20 DOI: 10.1016/j.susc.2024.122690

Baris Öcal, Philipp Weitkamp, Klaus Meerholz, Selina Olthof

{"title":"Chemical interaction and molecular growth of a highly dipolar merocyanine molecule on metal surfaces: A photoelectron spectroscopy study","authors":"Baris Öcal, Philipp Weitkamp, Klaus Meerholz, Selina Olthof","doi":"10.1016/j.susc.2024.122690","DOIUrl":"10.1016/j.susc.2024.122690","url":null,"abstract":"<div><div>The growth and ordering of molecules on surfaces is an intriguing research topic as insights gained here can be of significant relevance for organic electronic devices. While often simple, rigid molecules are employed as model systems, we show results for a highly dipolar merocyanine which is studied on top of Au(100), Ag(100) and Cu(100) metal single crystals. Film thicknesses ranging from sub-monolayer to multilayer regimes are analyzed using UV (UPS) and X-ray photoelectron spectroscopy (XPS). For the monolayer regime, there is strong indication of face-on orientation, with both of the molecules’ sulfur atoms bonding to the metal surfaces. Here, on Ag and Au(100) the sulfur atoms lose some or all of their intrinsic charges due to a charge transfer with the substrate, while on Cu(100) a strong metal-sulfur bond forms. The interaction between the substrate and the molecules can also be seen in the intensity and width of the highest occupied molecular orbital features in UPS. Upon multilayer deposition, a gradual lowering in ionization energy is observed, likely due to the formation of antiparallel dimers followed by an increased charge carrier delocalization due to the formation of an extended molecular aggregate for thicker layers. Interestingly, on Cu(100) the aggregated phase is already observed for much lower deposition, showing the importance of substrate-molecule interaction on the subsequent film growth. Therefore, this study offers a detailed understanding of the interface formation and electronic structure evolution for merocyanine films on different metal surfaces.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"754 ","pages":"Article 122690"},"PeriodicalIF":2.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

“Single-atom” catalysis: An opportunity for surface science

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-20 DOI: 10.1016/j.susc.2024.122687

Gareth S. Parkinson

{"title":"“Single-atom” catalysis: An opportunity for surface science","authors":"Gareth S. Parkinson","doi":"10.1016/j.susc.2024.122687","DOIUrl":"10.1016/j.susc.2024.122687","url":null,"abstract":"<div><div>Over the past decade, extensive research into ``single-atom'' catalysts (SACs) has revealed that the catalytic behavior of metal adatoms is highly dependent on how they interact with their support. A strong dependence on the local coordination environment has led to comparisons with metal-organic complexes, and there is growing excitement about the potential to fine-tune SACs by controlling the adsorption geometry. The rise of computational screening to identify the optimal support/metal combinations underscores the need for rigorous benchmarking of theoretical methods, to validate realistic geometries, mechanisms, and the impact of adsorption on stability and catalytic activity. The surface science approach is particularly well-suited for this task because it allows to precisely determine the geometry of the metal atom and interpret its catalytic behavior. Moreover, the effects of temperature and molecular adsorption on the model catalysts stability can be studied in isolation, and conclusions drawn from UHV studies tested in increasingly common near-ambient pressure and electrochemical setups. This perspective highlights recent breakthroughs and specific systems—including metal oxides, metal-organic frameworks, and carbon nitrides—where insights from surface science experiments can significantly advance understanding in this rapidly evolving field.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"754 ","pages":"Article 122687"},"PeriodicalIF":2.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151028","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

X-ray photoelectron diffraction as one efficient tool for surface structure determination of corrugated 2D materials

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-19 DOI: 10.1016/j.susc.2024.122683

Luis Henrique de Lima , Abner de Siervo

{"title":"X-ray photoelectron diffraction as one efficient tool for surface structure determination of corrugated 2D materials","authors":"Luis Henrique de Lima , Abner de Siervo","doi":"10.1016/j.susc.2024.122683","DOIUrl":"10.1016/j.susc.2024.122683","url":null,"abstract":"<div><div>This brief review discusses the application of X-ray photoelectron diffraction (XPD) as an effective experimental tool for determining the surface structure of two-dimensional (2D) corrugated materials, such as graphene and hexagonal boron nitride. XPD stands out for its ability to provide precise atomic positions, interlayer distances, bond lengths, and bond angles. Such detailed experimental data are essential for refining theoretical models and complement the findings obtained through other techniques, like scanning probe microscopy (SPM). This brief review includes examples of surface structure studies on sp<span><math><msup><mrow></mrow><mrow><mn>2</mn></mrow></msup></math></span>-hybridized corrugated monolayers, such as graphene on Ir(111), Fe-intercalated graphene on Ir(111), <span><math><mi>h</mi></math></span>BN on Rh(111), and graphene on SiC(0001). XPD has uncovered significant structural details, such as corrugation amplitude and adsorption distances to the substrate, contributing to an enhanced understanding of the electronic, mechanical, optical, magnetic, and physicochemical properties of 2D materials.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"754 ","pages":"Article 122683"},"PeriodicalIF":2.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Measurement of surface segregation via He+ ion scattering in CuxAgyAu1-x-y composition spread thin films

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-14 DOI: 10.1016/j.susc.2024.122682

Zhitao Guo , Robert A. Burnley , Andrew J. Gellman

{"title":"Measurement of surface segregation via He+ ion scattering in CuxAgyAu1-x-y composition spread thin films","authors":"Zhitao Guo , Robert A. Burnley , Andrew J. Gellman","doi":"10.1016/j.susc.2024.122682","DOIUrl":"10.1016/j.susc.2024.122682","url":null,"abstract":"<div><div>Surface segregation under UHV conditions was mapped out across Cu<em><sub>x</sub></em>Ag<em><sub>y</sub></em>Au<sub>1-</sub><em><sub>x</sub></em><sub>-</sub><em><sub>y</sub></em> (<em>x</em> = 0→1,<em>y</em> = 0→1‐x) composition space and over a temperature range of 500 – 800 K. E-beam deposition of Composition Spread Alloy Films (CSAFs), high-throughput SEM-EDX, XPS and LEIS experiments were performed to study the relationship between the alloy surface composition and bulk alloy composition. Strong depletion of Cu was observed across all alloy compositions, with <1 % surface Cu detected in alloys containing >20 % bulk Ag or >60 % bulk Au. The majority of the composition space is represented by AgAu surface alloys, showing weak Ag enrichment in alloys with low bulk Cu compositions (<25 % Ag enrichment) and significant Ag enrichment in alloys with higher Cu content (∼75 % Ag enrichment). Surface enrichment of Au in Cu was only observed in alloys with <5 % bulk Ag. These observations are quantitatively consistent with prior studies of the relevant binary alloys and qualitatively consistent with surface segregation driven by differences in surface energies. Alloys with surface Cu greater than 1 % were found to have temperature dependent segregation, varying by as much as 15 % surface Cu over the temperature range 500 – 800 K, while all other alloys showed negligible differences.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"754 ","pages":"Article 122682"},"PeriodicalIF":2.1,"publicationDate":"2024-12-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A first-principles study of hydrazine adsorption and decomposition on Pt(111) surface: The effect of partially dissociative H2O on decomposition process

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-12 DOI: 10.1016/j.susc.2024.122680

Yaolin Zhao , Dayin Tong , Zhongcun Chen , Songtao Xiao

{"title":"A first-principles study of hydrazine adsorption and decomposition on Pt(111) surface: The effect of partially dissociative H2O on decomposition process","authors":"Yaolin Zhao , Dayin Tong , Zhongcun Chen , Songtao Xiao","doi":"10.1016/j.susc.2024.122680","DOIUrl":"10.1016/j.susc.2024.122680","url":null,"abstract":"<div><div>Density functional theory with dispersion correction (DFT-D3) is used to investigate the adsorption and decomposition of hydrazine (N<sub>2</sub>H<sub>4</sub>) on Pt(111) surface, and the effect of water on decomposition process is considered. The stable adsorption configurations and adsorption energies are obtained for hydrazine, water and intermediate species. The hydrazine decomposition is investigated in three kinds of pathways including intramolecular dehydrogenation and intermolecular dehydrogenation via H atom or OH group assistance. It is shown that the adsorption of water in partially dissociative conformation (H and OH radicals) is the most stable on Pt(111) surface for its largest adsorption energy. The OH group can greatly promote the decomposition of hydrazine by drastically decreasing the energy barriers of dehydrogenation reactions, which are closely related to the overall PDOS distribution shifts of their transition states. From thermodynamics and kinetics points of view, the favorable decomposition pathway of hydrazine may be N<sub>2</sub>H<sub>4</sub>+OH→N<sub>2</sub>H<sub>3</sub>+OH→NHNH+OH→NNH+OH→N<sub>2</sub>.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"754 ","pages":"Article 122680"},"PeriodicalIF":2.1,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143150991","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Efficient parameterization of adsorbate–adsorbate interactions on metal surfaces

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-12 DOI: 10.1016/j.susc.2024.122678

Willem Vanmoerkerke, Rasmus Svensson, Henrik Grönbeck

引用次数: 0

The chemistry of bimetallic surfaces – Evolution of an atomic-scale picture

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-03 DOI: 10.1016/j.susc.2024.122677

R. Jürgen Behm, Axel Groß

引用次数: 0

Density functional theory study on the electrocatalytic performance of defected monolayer vanadium diselenide for oxygen evolution and reduction reactions

IF 2.1 4区化学

Surface Science Pub Date : 2024-12-01 DOI: 10.1016/j.susc.2024.122669

Rabia Hassan , Rehan Hassan , Fei Ma

{"title":"Density functional theory study on the electrocatalytic performance of defected monolayer vanadium diselenide for oxygen evolution and reduction reactions","authors":"Rabia Hassan , Rehan Hassan , Fei Ma","doi":"10.1016/j.susc.2024.122669","DOIUrl":"10.1016/j.susc.2024.122669","url":null,"abstract":"<div><div>The slow oxygen evolution reaction (OER) in the water-splitting driven by electricity, significantly impedes the hydrogen evolution reaction (HER). In this paper, density functional theory with D3 correction (DFT-D3) is utilized to explore the electrocatalytic potential of defected mono-layered VSe<sub>2</sub> for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Intrinsic point defects, such as, selenium (D1) and vanadium (D2) vacancies, are introduced into 2D-VSe<sub>2</sub>. Possible sites, like, Se Top, V Top, vacancies and bridge positions are investigated for OER and ORR intermediates (O, OH and OOH). VSe<sub>2</sub> monolayer with V vacancy (D2) shows significantly reduced overpotential for OER/ORR (η= 0.19 V/0.46 V), indicating enhanced catalytic activity. The OER performances of VSe<sub>2</sub> monolayer with V vacancy (D2) (η= 0.19 V) surpasses those of IrO<sub>2</sub> and RuO<sub>2</sub> (η= 0.37 V and 0.56 V), and the ORR performances (η= 0.46 V) are comparable to those of precious Pt (η=0.4 V). The Pourbaix diagram further confirms the aqueous stability of VSe<sub>2</sub> in various pH environments, establishing its potential as a robust catalyst for OER and ORR. These findings suggest that defect engineering, particularly vanadium vacancies, could significantly improve the electrocatalytic activity of VSe<sub>2</sub> monolayers, contributing to the development of high-performance electrocatalysts.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"754 ","pages":"Article 122669"},"PeriodicalIF":2.1,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143150989","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0