Surface Science最新文献_第7页

Measurement of surface segregation via He+ ion scattering in CuxAgyAu1-x-y composition spread thin films 利用He+离子散射测量CuxAgyAu1-x-y成分扩散薄膜的表面偏析

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 Pt（111）表面联氨吸附分解的第一性原理研究：部分解离水对分解过程的影响

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 金属表面吸附物-吸附物相互作用的有效参数化

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 双金属表面的化学性质——原子尺度图像的演化

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 缺陷单层二硒化钒析氧还原电催化性能的密度泛函理论研究

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

Electronic reconfiguration induced by dynamic hydroxyl decoration facilitates electrochemical nitrate reduction to ammonia 动态羟基修饰引起的电子重构促进了硝酸盐的电化学还原为氨

IF 2.1 4区化学

Surface Science Pub Date : 2024-11-28 DOI: 10.1016/j.susc.2024.122668

Tinghui Li , Yun Shan , Lizhe Liu

引用次数: 0

Thermodynamic and kinetic analysis of the oxygen evolution reaction on TiO2 (100) and (101) surfaces: A DFT study 二氧化钛（100）和（101）表面析氧反应的热力学和动力学分析：DFT研究

IF 2.1 4区化学

Surface Science Pub Date : 2024-11-23 DOI: 10.1016/j.susc.2024.122654

Felipe Marinho Fernandes , Neubi Francisco Xavier Jr , Glauco Favilla Bauerfeldt , Márcio Soares Pereira , Clarissa Oliveira da Silva

{"title":"Thermodynamic and kinetic analysis of the oxygen evolution reaction on TiO2 (100) and (101) surfaces: A DFT study","authors":"Felipe Marinho Fernandes , Neubi Francisco Xavier Jr , Glauco Favilla Bauerfeldt , Márcio Soares Pereira , Clarissa Oliveira da Silva","doi":"10.1016/j.susc.2024.122654","DOIUrl":"10.1016/j.susc.2024.122654","url":null,"abstract":"<div><div>The search for alternative energy sources with sustained economic viability and minimal pollution is imperative, making hydrogen a promising candidate as a fuel. This work provides important findings on the Oxygen Evolution Reactions (OER) on TiO<sub>2</sub>, with a focus on elucidating the reaction mechanisms. Density Functional Theory calculations were applied on both the (101) and (100) surfaces of the catalyst. The application of overpotentials was evaluated, with 2.85 and 2.32 eV required for (101) and (100) surface, respectively, for all reaction steps to be exergonic. The 0.53 eV difference suggests a potentially favorable pathway for the OER on the (100) surface. When evaluating the kinetics, an additional barrier of 2.84 eV under the <span><math><mrow><mi>U</mi><mo>=</mo><mn>0</mn><mo>.</mo><mn>00</mn></mrow></math></span> V condition on the (100) surface is found for the formation of the OOH intermediate, suggesting the kinetics preference for the oxygen evolution process on the (101) surface.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"753 ","pages":"Article 122654"},"PeriodicalIF":2.1,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142748419","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

CO–induced roughening of Cu(111): formation and detection of reactive nanoclusters on metal surfaces co诱导Cu（111）粗化：金属表面反应性纳米团簇的形成和检测

IF 2.1 4区化学

Surface Science Pub Date : 2024-11-22 DOI: 10.1016/j.susc.2024.122665

Konstantinos G. Papanikolaou , Lang Xu , Evangelos Smith , Manos Mavrikakis

{"title":"CO–induced roughening of Cu(111): formation and detection of reactive nanoclusters on metal surfaces","authors":"Konstantinos G. Papanikolaou , Lang Xu , Evangelos Smith , Manos Mavrikakis","doi":"10.1016/j.susc.2024.122665","DOIUrl":"10.1016/j.susc.2024.122665","url":null,"abstract":"<div><div>The formation of nanoclusters on metal surfaces in the presence of reactive environments is a phenomenon with important implications for catalysis. These nanoclusters are composed of atoms ejected from undercoordinated sites such as step edges, and their presence alters the catalytic properties of solid materials. We perform density functional theory (DFT) and kinetic Monte Carlo (KMC) simulations to investigate the formation and reactivity of copper clusters on Cu(111). Our results indicate a considerably higher reactivity of small copper nanoclusters, with up to seven atoms in size on roughened copper surfaces than on pristine Cu(111) and Cu(211). Regarding the restructuring events that give rise to nanoclusters under CO atmospheres, we determine that the ejection of Cu atoms from step edges and their migration therefrom to adjacent Cu(111) terraces are, by and large, driven by CO coverage effects. By means of KMC simulations, which account for CO–CO lateral interactions and CO–induced surface restructuring, we show that temperature programmed desorption (TPD) holds promise for the detection of highly reactive nanoclusters. Our approach showcases how surface restructuring and surface–adsorbate bond breaking can be combined when modeling surface reactions and contributes to the development of an advanced understanding of the nature of active site under reaction conditions.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"754 ","pages":"Article 122665"},"PeriodicalIF":2.1,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143151722","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

Surface science study on catalytic surfaces under working conditions with soft-X-ray surface spectroscopy at the Photon Factory 在光子工厂利用软 X 射线表面光谱对工作条件下的催化表面进行表面科学研究

IF 2.1 4区化学

Surface Science Pub Date : 2024-11-21 DOI: 10.1016/j.susc.2024.122657

Hiroshi Kondoh

{"title":"Surface science study on catalytic surfaces under working conditions with soft-X-ray surface spectroscopy at the Photon Factory","authors":"Hiroshi Kondoh","doi":"10.1016/j.susc.2024.122657","DOIUrl":"10.1016/j.susc.2024.122657","url":null,"abstract":"<div><div>This minireview provides an overview of recent advancements in <em>in situ/operando</em> soft X-ray surface spectroscopy, particularly focusing on the development and application of techniques such as near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and soft X-ray absorption spectroscopy (SXAS) conducted at the Photon Factory. These techniques enable us to observe catalytic surfaces under working conditions, which provides new insights into catalytic mechanisms by probing the chemical states of reactive species as well as catalytic surfaces. The review highlights three case studies: the reduction of nitrogen oxide (NO) on rhodium (Rh) catalysts, ethylene epoxidation on silver (Ag) catalysts, and water-splitting photocatalysis using SrTiO<sub>3</sub> with co-catalysts. Each study shows how these techniques reveal critical aspects about surface reactions, structures of intermediate species, and photoinduced processes, which contributes to a deeper understanding of reactive species and reaction pathways. I also discuss about the challenges in <em>operando</em> kinetic analyses, structure analyses and extension of applicable catalytic phenomena and suggest future improvements in <em>operando</em> spectroscopy to enhance the capability of these analyses.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"753 ","pages":"Article 122657"},"PeriodicalIF":2.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142722420","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

Time-resolved ambient pressure x-ray photoelectron spectroscopy: Advancing the operando study of ALD chemistry 时间分辨环境压力x射线光电子能谱：推进ALD化学操作的研究

IF 2.1 4区化学

Surface Science Pub Date : 2024-11-20 DOI: 10.1016/j.susc.2024.122656

Rosemary Jones , Esko Kokkonen , Calley Eads , Ulrike K. Küst , Julia Prumbs , Jan Knudsen , Joachim Schnadt

{"title":"Time-resolved ambient pressure x-ray photoelectron spectroscopy: Advancing the operando study of ALD chemistry","authors":"Rosemary Jones , Esko Kokkonen , Calley Eads , Ulrike K. Küst , Julia Prumbs , Jan Knudsen , Joachim Schnadt","doi":"10.1016/j.susc.2024.122656","DOIUrl":"10.1016/j.susc.2024.122656","url":null,"abstract":"<div><div>Today, atomic layer deposition (ALD) has become a firm corner stone of thin film deposition technology. The microelectronics industry, an early adopter of ALD, imposes stringent requirements on ALD to produce films with highly defined physical and chemical properties, which becomes even more important as device and component dimensions decrease. This, in turn, means that our understanding of the chemical processes underlying ALD needs to increase exponentially. Here, we show that one can use synchrotron-based time-resolved ambient pressure x-ray photoelectron spectroscopy (APXPS) to obtain highly detailed <em>operando</em> information on the surface chemistry of ALD, not only, as proven earlier, during the initial ALD cycles, but also for the steady-growth regime reached during the later stages of deposition. Using event averaging and Fourier-transform methods, we show that the ALD of TiO<sub>2</sub> from titanium tetraisopropoxide (TTIP) and water precursors in the steady-growth regime follows the suggested ligand-exchange reaction mechanism, with no sign of oxygen transport between the deposited layers and the bulk of the film, as has been observed for other materials systems. Hence, the TiO<sub>2</sub> ALD from TTIP and water constitutes a textbook example of metal oxide ALD, as expected for this well-known ALD process. The detailed insight is made possible by computerised control of the precursor pulses that enable the recording of long data sets, which comprise many ALD cycles at highly regular intervals, in combination with an advanced data analysis that allows us to pick out signals undetectable in the raw data. The analysis method also allows to separate oscillating contributions to the signals induced by the ALD pulsing from the overwhelming bulk signal.</div></div>","PeriodicalId":22100,"journal":{"name":"Surface Science","volume":"753 ","pages":"Article 122656"},"PeriodicalIF":2.1,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142748421","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