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Experimental and theoretical studies of reaction pathways of direct propylene epoxidation on model catalyst surfaces 模型催化剂表面丙烯直接环氧化反应途径的实验与理论研究
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2021-05-01 DOI: 10.1016/j.surfrep.2021.100524
William N. Porter, Zhexi Lin, Jingguang G. Chen
{"title":"Experimental and theoretical studies of reaction pathways of direct propylene epoxidation on model catalyst surfaces","authors":"William N. Porter,&nbsp;Zhexi Lin,&nbsp;Jingguang G. Chen","doi":"10.1016/j.surfrep.2021.100524","DOIUrl":"https://doi.org/10.1016/j.surfrep.2021.100524","url":null,"abstract":"<div><p><span><span><span>The direct epoxidation of </span>propylene to propylene oxide (PO) using </span>molecular oxygen<span> is an attractive alternative to current production methods using chlorohydrin or hydroperoxide-mediated processes, which are environmentally harmful and expensive. Although direct ethylene epoxidation using Ag-based catalysts has been practiced industrially for decades, due to the presence of allylic hydrogen in propylene the selectivity<span> toward epoxide is generally much lower for propylene than for ethylene. Mechanistic understanding on well-characterized surfaces of model catalysts can potentially provide guidance to effectively alter the electronic properties of the catalyst in order to increase PO selectivity. This review summarizes both experimental and theoretical studies on model catalysts for propylene epoxidation and their contributions to elucidating the reaction mechanism, intermediates, and active sites. We first show examples of experimental studies on Cu, Ag, and Au surfaces, and compare the reaction pathways and intermediates on these surfaces. Novel approaches including plasmon-mediated catalysis and utilization of shape-controlled crystal facets that open new opportunities for improving PO selectivity will also be discussed. We then describe how </span></span></span>density functional theory<span> (DFT) calculations have provided important insights into the reaction mechanism and active sites on Cu, Ag, and Au surfaces and clusters. Propylene oxidation<span> pathways on other relevant metal surfaces will also be discussed. The combined experimental and computational studies elucidate the nature of surface oxygen species and the role of the oxametallacycle intermediate. We conclude by highlighting design principles and insights for guiding further development of active and selective propylene epoxidation catalysts.</span></span></p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"76 2","pages":"Article 100524"},"PeriodicalIF":9.8,"publicationDate":"2021-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2021.100524","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2186996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 10
Synthesis and characterization of 2D transition metal dichalcogenides: Recent progress from a vacuum surface science perspective 二维过渡金属二硫族化合物的合成与表征:真空表面科学的最新进展
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2021-05-01 DOI: 10.1016/j.surfrep.2021.100523
Kinga Lasek , Jingfeng Li , Sadhu Kolekar , Paula Mariel Coelho , Lu'an Guo , Min Zhang , Zhiming Wang , Matthias Batzill
{"title":"Synthesis and characterization of 2D transition metal dichalcogenides: Recent progress from a vacuum surface science perspective","authors":"Kinga Lasek ,&nbsp;Jingfeng Li ,&nbsp;Sadhu Kolekar ,&nbsp;Paula Mariel Coelho ,&nbsp;Lu'an Guo ,&nbsp;Min Zhang ,&nbsp;Zhiming Wang ,&nbsp;Matthias Batzill","doi":"10.1016/j.surfrep.2021.100523","DOIUrl":"https://doi.org/10.1016/j.surfrep.2021.100523","url":null,"abstract":"&lt;div&gt;&lt;p&gt;&lt;span&gt;&lt;span&gt;Layered transition metal dichalcogenides&lt;span&gt; (TMDs) are a diverse group of materials whose properties vary from semiconducting to metallic with a variety of many body phenomena, ranging from charge density wave (CDW), &lt;/span&gt;&lt;/span&gt;superconductivity&lt;span&gt;&lt;span&gt;, to Mott-insulators. Recent interest in topologically protected states revealed also that some TMDs host bulk Dirac- or Wyle-semimetallic states and their corresponding surface states. In this review, we focus on the synthesis of TMDs by vacuum processes, such as molecular beam epitaxy&lt;span&gt; (MBE). After an introduction of these preparation methods and categorize the basic electronic properties of TMDs, we address the characterization of vacuum synthesized materials in their ultrathin limit-mainly as a single monolayer material. Scanning tunneling microscopy and angle resolved &lt;/span&gt;&lt;/span&gt;photoemission&lt;span&gt;&lt;span&gt; spectroscopy has revealed detailed information on how monolayers differ in their properties from multi-layer and bulk materials. The status of monolayer properties is given for the TMDs, where data are available. Distinct modifications of monolayer properties compared to their bulk counterparts are highlighted. This includes the well-known transition from indirect to direct band gap in semiconducting group VI-B TMDs as the material-thickness is reduced to a single &lt;/span&gt;molecular layer. In addition, we discuss the new or modified CDW states in monolayer VSe&lt;/span&gt;&lt;/span&gt;&lt;/span&gt;&lt;sub&gt;2&lt;/sub&gt; and TiTe&lt;sub&gt;2&lt;/sub&gt;, a Mott-insulating state in monolayer 1T-TaSe&lt;sub&gt;2&lt;/sub&gt;&lt;span&gt;, and the monolayer specific 2D topological insulator 1T′-WTe&lt;/span&gt;&lt;sub&gt;2&lt;/sub&gt;, which gives rise to a quantum spin Hall insulator. New structural phases, that do not exist in the bulk, may be synthesized in the monolayer by MBE. These phases have special properties, including the Mott insulator 1T-NbSe&lt;sub&gt;2&lt;/sub&gt;&lt;span&gt;, the 2D topological insulators of 1T′-MoTe&lt;/span&gt;&lt;sub&gt;2&lt;/sub&gt;, and the CDW material 1T-VTe&lt;sub&gt;2&lt;/sub&gt;&lt;span&gt;&lt;span&gt;. After discussing the pure&lt;span&gt; TMDs, we report the properties of nanostructured or modified TMDs. Edges and mirror twin grain boundaries (MTBs) in 2D materials are 1D structures. In group VI-B semiconductors, these 1D structures may be metallic and their properties obey Tomonaga Luttinger quantum liquid behavior. Formation of Mo-rich MTBs in Mo-dichalcogenides and self-intercalation in between TMD-layers are discussed as potential compositional variants that may occur during MBE synthesis of TMDs or may be induced intentionally during post-growth modifications. In addition to compositional modifications, &lt;/span&gt;&lt;/span&gt;phase switching&lt;span&gt; and control, in particular between the 1H and 1T (or 1T′) phases, is a recurring theme in TMDs. Methods of phase control by tuning growth conditions or by post-growth modifications, e.g. by electron doping, are discussed. The properties of heterostructures&lt;span&gt;&lt;span&gt; of TMD monolayers are also introduced, with a focus ","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"76 2","pages":"Article 100523"},"PeriodicalIF":9.8,"publicationDate":"2021-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2021.100523","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2344304","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 39
Adsorption and valence electronic states of nitric oxide on metal surfaces 金属表面一氧化氮的吸附和价电子态
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2021-03-01 DOI: 10.1016/j.surfrep.2020.100500
Akitoshi Shiotari , Hiroyuki Koshida , Hiroshi Okuyama
{"title":"Adsorption and valence electronic states of nitric oxide on metal surfaces","authors":"Akitoshi Shiotari ,&nbsp;Hiroyuki Koshida ,&nbsp;Hiroshi Okuyama","doi":"10.1016/j.surfrep.2020.100500","DOIUrl":"https://doi.org/10.1016/j.surfrep.2020.100500","url":null,"abstract":"<div><p>Among fundamental diatomic molecules<span><span>, the adsorption of carbon monoxide (CO) and </span>nitric oxide<span><span><span><span> (NO) on metal surfaces has been a subject of intensive research in the </span>surface science<span> community, partly owing to its relevance to heterogeneous catalysis used for environmental control. Compared to the rather well-defined adsorption mechanism of CO, that of NO is less understood because the adsorption results in much more </span></span>complex reactions<span>. The complexity is ascribed to the open-shell structure of valence electrons, making the molecule readily interact with the metal surface itself as well as with co-adsorbed molecules. Furthermore, the interaction crucially depends on the local structure of the surface. Therefore, to elucidate the interaction at the molecular scale, it is essential to study the valence state as well as the bonding geometry for individual NO molecules placed in a well-defined environment on the surface. Scanning tunneling microscopy (STM) is suitable for this purpose. In this review, we summarize the knowledge about the interaction of NO with metal surfaces, mainly focused on the valence electronic states, followed by recent studies using STM and </span></span>atomic force microscopy (AFM) at the level of individual molecules.</span></span></p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"76 1","pages":"Article 100500"},"PeriodicalIF":9.8,"publicationDate":"2021-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2020.100500","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1945435","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 9
Noncontact atomic force microscopy: Bond imaging and beyond 非接触原子力显微镜:键成像及其他
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2020-11-01 DOI: 10.1016/j.surfrep.2020.100509
Qigang Zhong , Xuechao Li, Haiming Zhang, Lifeng Chi
{"title":"Noncontact atomic force microscopy: Bond imaging and beyond","authors":"Qigang Zhong ,&nbsp;Xuechao Li,&nbsp;Haiming Zhang,&nbsp;Lifeng Chi","doi":"10.1016/j.surfrep.2020.100509","DOIUrl":"https://doi.org/10.1016/j.surfrep.2020.100509","url":null,"abstract":"<div><p>It was a long-cherished dream for chemists to take a direct look at chemical bonding, a fundamental component of chemistry<span>. This dream was finally accomplished by the state-of-the-art noncontact atomic force microscopy<span><span> (NC-AFM) equipped with qPlus force sensors and carbon monoxide (CO) functionalized tips. The resolved interconnectivity between atoms and molecules in NC-AFM frequency shift images is interpreted as chemical bonding, providing essential knowledge of the bond length, </span>bond angle<span><span> and even bond order. The featured contrast of different chemical bonds can serve as fingerprints for further interpretation of chemical structures<span> toward unknown species synthesized on surfaces. This breakthrough enriches characterization tools for surface science<span> and brings our understanding of on-surface reactions to a new level. Beyond bond imaging, the application of NC-AFM has been extended to quantifying interatomic interactions, identifying three-dimensional nanostructures, manipulating molecules and reactions, as well as determining </span></span></span>molecular electronic<span><span> characteristics. Moreover, some recent efforts address the improvement of the usability and versatility of the bond-resolved NC-AFM technique, including high-resolution molecular investigation on bulk insulators, application-specific tip modification, stable bond imaging above </span>liquid helium temperature and autonomous experimentation implemented by artificial intelligence.</span></span></span></span></p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"75 4","pages":"Article 100509"},"PeriodicalIF":9.8,"publicationDate":"2020-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2020.100509","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1847966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 18
Synchrotron infrared nano-spectroscopy and -imaging 同步加速器红外纳米光谱学与成像
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2020-08-01 DOI: 10.1016/j.surfrep.2020.100493
Hans A. Bechtel , Samuel C. Johnson , Omar Khatib , Eric A. Muller , Markus B. Raschke
{"title":"Synchrotron infrared nano-spectroscopy and -imaging","authors":"Hans A. Bechtel ,&nbsp;Samuel C. Johnson ,&nbsp;Omar Khatib ,&nbsp;Eric A. Muller ,&nbsp;Markus B. Raschke","doi":"10.1016/j.surfrep.2020.100493","DOIUrl":"https://doi.org/10.1016/j.surfrep.2020.100493","url":null,"abstract":"<div><p><span><span><span>Infrared (IR) spectroscopy has evolved into a powerful analytical technique to probe molecular and </span>lattice vibrations<span><span>, low-energy electronic excitations and correlations, and related collective </span>surface plasmon<span>, phonon<span><span>, or other polaritonic resonances. In combination with scanning probe microscopy, near-field infrared nano-spectroscopy and -imaging techniques have recently emerged as a frontier in imaging science, enabling the study of complex heterogeneous materials with simultaneous </span>nanoscale spatial resolution and chemical and quantum state spectroscopic specificity. Here, we describe </span></span></span></span>synchrotron<span> infrared nano-spectroscopy (SINS), which takes advantage of the low-noise, broadband, high spectral irradiance, and coherence of synchrotron infrared radiation for near-field infrared measurements across the mid- to far-infrared with nanometer spatial resolution. This powerful combination provides a qualitatively new form of broadband spatio-spectral analysis of nanoscale, mesoscale, and surface phenomena that were previously difficult to study with IR techniques, or even any form of micro-spectroscopy in general. We review the development of SINS, describe its technical implementations, and highlight selected examples representative of the rapidly growing range of applications in physics, </span></span>chemistry, biology, materials science, geology, and atmospheric and space sciences.</p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"75 3","pages":"Article 100493"},"PeriodicalIF":9.8,"publicationDate":"2020-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2020.100493","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2186997","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 26
Wettability of graphene 石墨烯的润湿性
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2020-05-01 DOI: 10.1016/j.surfrep.2020.100482
Liubov A. Belyaeva, Grégory F. Schneider
{"title":"Wettability of graphene","authors":"Liubov A. Belyaeva,&nbsp;Grégory F. Schneider","doi":"10.1016/j.surfrep.2020.100482","DOIUrl":"https://doi.org/10.1016/j.surfrep.2020.100482","url":null,"abstract":"<div><p>Many far-reaching applications of graphene require a deep understanding of the interactions between graphene and other surfaces, including the wetting behaviour of graphene. However, its two-dimensional nature does not allow qualifying graphene as simply hydrophobic or hydrophilic, but instead gives rise to a diversity of interfacial phenomena governing the apparent wettability of graphene. As a result, wide disparities in the wetting properties of graphene have been widely reported. In this review we analyse the wettability of graphene with a special focus on the experimental conditions and on discriminating the causes of the reported inconsistencies. The elimination of the environmental factors causing misleading data is a major challenge. Importantly, progresses made in graphene research yielded new experimental insights and tools enabling the minimization of unwanted effects and, ultimately, the achievement of reliable contact angle measurements. Besides the macroscopic wettability studied using contact angle measurements under ambient conditions or by theoretical modelling, we also analysed correlations with the wettability of graphene at the molecular level in supremely pure environment of ultra-high vacuum.</p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"75 2","pages":"Article 100482"},"PeriodicalIF":9.8,"publicationDate":"2020-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2020.100482","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2402363","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 45
The electrochemical interface in first-principles calculations 第一性原理计算中的电化学界面
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2020-05-01 DOI: 10.1016/j.surfrep.2020.100492
Kathleen Schwarz , Ravishankar Sundararaman
{"title":"The electrochemical interface in first-principles calculations","authors":"Kathleen Schwarz ,&nbsp;Ravishankar Sundararaman","doi":"10.1016/j.surfrep.2020.100492","DOIUrl":"https://doi.org/10.1016/j.surfrep.2020.100492","url":null,"abstract":"<div><p><span>First-principles predictions play an important role in understanding chemistry<span><span> at the electrochemical interface. Electronic structure calculations are straightforward for vacuum interfaces, but do not easily account for the interfacial fields and </span>solvation<span> that fundamentally change the nature of electrochemical reactions. Prevalent techniques for first-principles prediction of electrochemical processes range from expensive explicit solvation using </span></span></span><em>ab initio</em><span><span> molecular dynamics, through a hierarchy of continuum solvation techniques, to neglecting solvation and interfacial field effects entirely. Currently, no single approach reliably captures all relevant effects of the </span>electrochemical double layer in first-principles calculations.</span></p><p><span>This review systematically lays out the relation between all major approaches to first-principles electrochemistry, including the key approximations and their consequences for accuracy and computational cost. Focusing on </span><em>ab initio</em> methods for thermodynamic properties of aqueous interfaces, we first outline general considerations for modeling electrochemical interfaces, including solvent and electrolyte dynamics and electrification. We then present the specifics of various explicit and implicit models of the solvent and electrolyte. Finally, we discuss the compromise between computational efficiency and accuracy, and identify key outstanding challenges and future opportunities in the wide range of techniques for first-principles electrochemistry.</p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"75 2","pages":"Article 100492"},"PeriodicalIF":9.8,"publicationDate":"2020-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2020.100492","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"1847967","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 71
Non-covalent interaction controlled 2D organic semiconductor films: Molecular self-assembly, electronic and optical properties, and electronic devices 非共价相互作用控制的二维有机半导体薄膜:分子自组装,电子和光学性质,以及电子器件
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2020-05-01 DOI: 10.1016/j.surfrep.2020.100481
Jia Lin Zhang , Xin Ye , Chengding Gu , Cheng Han , Shuo Sun , Li Wang , Wei Chen
{"title":"Non-covalent interaction controlled 2D organic semiconductor films: Molecular self-assembly, electronic and optical properties, and electronic devices","authors":"Jia Lin Zhang ,&nbsp;Xin Ye ,&nbsp;Chengding Gu ,&nbsp;Cheng Han ,&nbsp;Shuo Sun ,&nbsp;Li Wang ,&nbsp;Wei Chen","doi":"10.1016/j.surfrep.2020.100481","DOIUrl":"https://doi.org/10.1016/j.surfrep.2020.100481","url":null,"abstract":"<div><p><span><span>The establishment of electronic and opto-electronic products relying on organic semiconductors (OSCs) has been intensely explored over the past few decades due to their great competitiveness in large area, low cost, flexible, wearable and </span>implantable devices<span>. Many of these products already entered our daily lives, such as organic light-emitting diodes-based displays, portable organic solar cells<span> and organic field-effect transistors. The device performance of OSC devices are determined by the supramolecular organization (orientation, morphology) as well as the supramolecular organization dependent energy level alignment at various interfaces (organic/electrode, organic/dielectric, organic/organic). This review focuses on the impact of non-covalent interaction on the molecular self-assembly of organic thin films<span>, their electronic and optical properties, as well as the device performance. Beginning with the growth of multiple OSCs on substrates with different interfacial interaction </span></span></span></span>strengths<span><span><span> (metals, insulators, semiconductors), the critical roles of molecule-substrate and </span>intermolecular interactions in determining the thin film organization have been demonstrated. Several non-covalent interactions that contribute to the energy levels of organic materials in solid phase are summarized, mainly including the induction contributions, </span>electrostatic interactions, band dispersions and interface dipoles. The excitonic coupling in specific aggregations of organic molecules and the corresponded effect on their optical properties are also discussed. Finally, the influences of weak intermolecular interactions on the device performance are presented.</span></p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"75 2","pages":"Article 100481"},"PeriodicalIF":9.8,"publicationDate":"2020-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2020.100481","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2484822","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 19
Vibrational Raman spectroscopy on adsorbate-induced low-dimensional surface structures 吸附诱导低维表面结构的振动拉曼光谱
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2020-03-01 DOI: 10.1016/j.surfrep.2020.100480
Eugen Speiser , Norbert Esser , Benedikt Halbig , Jean Geurts , Wolf Gero Schmidt , Simone Sanna
{"title":"Vibrational Raman spectroscopy on adsorbate-induced low-dimensional surface structures","authors":"Eugen Speiser ,&nbsp;Norbert Esser ,&nbsp;Benedikt Halbig ,&nbsp;Jean Geurts ,&nbsp;Wolf Gero Schmidt ,&nbsp;Simone Sanna","doi":"10.1016/j.surfrep.2020.100480","DOIUrl":"https://doi.org/10.1016/j.surfrep.2020.100480","url":null,"abstract":"<div><p>Low-dimensional self-organized surface structures, induced by (sub)monolayer metal adsorbates on semiconductor surfaces may give rise not only to a variety of emergent electronic properties, but also to a multitude of specific localized vibronic features. The focus of this review is on the analysis of these novel surface vibration eigenmodes. The application of <em>in situ</em> surface Raman spectroscopy under UHV conditions on clean semiconductor surfaces and those with self-ordered adsorbates, in close conjunction with the calculations of Raman spectra, based on the first-principles determination of the structural, electronic and vibronic properties, allows a consistent determination of the vibration eigenfrequencies, symmetry properties, and elongation patterns of the systems of interest. The localized nature of the surface eigenmodes determines the surface sensitivity, independent of the large penetration depth of light. The surface contribution can be selectively enhanced by employing resonance conditions to surface electronic transitions. Moreover, surface and bulk contributions can be separated by taking difference spectra between various stages of surface preparation. The relevant surfaces are Ge and especially Si with different orientations ((111) and vicinal (hhk)), on which the adsorption of various metals (Au, Sn, Pb, or In) gives rise to two- and quasi-one-dimensional structures (e.g. Au-(5 × 2)/Si(111)) with a variety of vibration modes. The Raman analysis of these modes not only enables the distinction between different proposed structural models (e.g. for Au-(<span><math><msqrt><mrow><mn>3</mn></mrow></msqrt><mo>×</mo><msqrt><mrow><mn>3</mn></mrow></msqrt></math></span>)/Si(111)), but also gives access to the role of electron-phonon coupling in structural phase transitions (e.g. for In-(8 × 2)–(4 × 1)/Si(111)).</p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"75 1","pages":"Article 100480"},"PeriodicalIF":9.8,"publicationDate":"2020-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2020.100480","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"2186999","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 3
Surface chemistry and catalysis of oxide model catalysts from single crystals to nanocrystals 氧化物模型催化剂从单晶到纳米晶的表面化学和催化作用
IF 9.8 1区 化学
Surface Science Reports Pub Date : 2019-11-01 DOI: 10.1016/j.surfrep.2019.100471
Shilong Chen , Feng Xiong , Weixin Huang
{"title":"Surface chemistry and catalysis of oxide model catalysts from single crystals to nanocrystals","authors":"Shilong Chen ,&nbsp;Feng Xiong ,&nbsp;Weixin Huang","doi":"10.1016/j.surfrep.2019.100471","DOIUrl":"https://doi.org/10.1016/j.surfrep.2019.100471","url":null,"abstract":"<div><p><span>Fundamental understandings of surface chemistry and catalysis of solid catalysts are of great importance for the developments of efficient catalysts and corresponding catalytic processes, but have been remaining as a challenge due to the complex nature of heterogeneous catalysis<span>. Model catalysts approach based on catalytic materials with uniform and well-defined surface structures is an effective strategy. Single crystals-based model catalysts have been successfully used for surface chemistry studies of solid catalysts, but encounter the so-called “materials gap” and “pressure gap” when applied for catalysis studies of solid catalysts. Recently catalytic nanocrystals with uniform and well-defined surface structures have emerged as a novel type of model catalysts whose surface chemistry and catalysis can be studied under the same operational reaction condition as working powder catalysts, and they are recognized as a novel type of model catalysts that can bridge the “materials gap” and “pressure gap” between single crystals-based model catalysts and powder catalysts. Herein we review recent progress of surface chemistry and catalysis of important oxide catalysts including CeO</span></span><sub>2</sub>, TiO<sub>2</sub> and Cu<sub>2</sub>O acquired by model catalysts from single crystals to nanocrystals with an aim at summarizing the commonalities and discussing the differences among model catalysts with complexities at different levels. Firstly, the complex nature of surface chemistry and catalysis of solid catalysts is briefly introduced. In the following sections, the model catalysts approach is described and surface chemistry and catalysis of CeO<sub>2</sub>, TiO<sub>2</sub> and Cu<sub>2</sub>O single crystal and nanocrystal model catalysts are reviewed. Finally, concluding remarks and future prospects are given on a comprehensive approach of model catalysts from single crystals to nanocrystals for the investigations of surface chemistry and catalysis of powder catalysts approaching the working conditions as closely as possible.</p></div>","PeriodicalId":434,"journal":{"name":"Surface Science Reports","volume":"74 4","pages":"Article 100471"},"PeriodicalIF":9.8,"publicationDate":"2019-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1016/j.surfrep.2019.100471","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"3263785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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: 85
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