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Applications of in-situ wide spectral range infrared absorption spectroscopy for CO oxidation over Pd/SiO_(2) and Cu/SiO_(2) catalysts

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Chinese Journal of Catalysis 2022年第8期43卷 2001-2009页

作者： Xuefei Weng Shuangli Yang Ding Ding Mingshu Chen Huilin Wan State Key laboratory of Physical Chemistry of Solid surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina Vacuum Interconnected nanotech Workstation Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123JiangsuChina

Infrared(IR)absorption spectroscopy has been widely used for dynamic characterization of catalysts and mechanism of catalytic ***,due to the strong infrared absorption of heterogeneous catalysts(mainly oxides,or supported metal and metal oxides,etc.)below 1200 cm^(-1),and the intensity of regular infrared light source rapidly decays at low-wavenumber range,most in-situ infrared spectroscopy studies are limited to the detection of surface adsorbates in the range of 4000-900 cm^(-1).The change of catalytically active component itself(M-O,M-M bond,etc.,1200-50 cm^(-1))during the reaction is hard to be tracked under reaction conditions by in-situ *** this work,a home-made in-situ IR reactor was designed and a sample preparing method was *** such progresses,the changes of reactants,products,surface adsorbates,and catalysts themselves can be measured under the same reaction conditions with a spectral range of 4000-400 cm^(-1),providing a new opportunity for in-situ characterization of heterogeneous *** oxidation on Pd/SiO_(2) and Cu/SiO_(2) catalysts were taken as examples,since both the two catalytic systems were extensively used commercially,and moreover reduction and oxidation of palladium and copper occur during the examined reaction *** characteristic bands of Pd^(2+)-O(670,608 cm^(-1)),Cu^(+)-O(635 cm^(-1))and Cu^(2+)-O(595,535 cm^(-1))were observed by IR,and the changes during CO oxidation reaction were successfully monitored by *** oxidation/reduction of palladium and copper were also confirmed by ex-situ ***,Pd^(0) in Pd/SiO_(2) and Cu^(+)in Cu/SiO_(2) were found as the thermal dynamically stable phases under the examined conditions for CO oxidation.

关键词： In-situ infrared spectroscopy X-ray photoelectron spectroscopy Heterogeneous catalysis CO oxidation Palladium Copper

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Superhydrophobic surfaces Produced by Applying a Self- Assembled Monolayer to Silicon Micro/Nano-Textured surfaces

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Nano Research 2009年第2期2卷 143-150页

作者： Yong Song Rahul Premachandran Nair Min Zou Yongqiang Wang Department of Mechanical Engineering University of ArkansasFayettevilleAR 72701USA Ocean nanotech LLC.2143 Worth LaneSpringdaleAR 72764USA

A novel way of producing superhydrophobic surfaces by applying a self-assembled monolayer(SAM)to silicon micro/nano-textured surfaces is presented in this *** micro/nano-textured surfaces on silicon substrates were generated by the aluminum-induced crystallization(AIC)of amorphous silicon(a-Si)***(OTS)SAMs were then applied to the textured surfaces by dip *** topography and wetting properties of the resulting surfaces were characterized using scanning electron microscopy(SEM)and a video-based contact angle measurement *** results show that by introducing OTS SAMs on the silicon micro/nano-textured surfaces,superhydrophobic surfaces with water contact angles(WCAs)of 155°were obtained,as compared to the WCAs of OTS-modified smooth silicon surfaces of about 112°.Surface topography was found to directly influence the WCA as predicted by the Cassie-Baxter model.

关键词： Superhydrophobic wetting property micro/nano-textured surfaces octadecyltrichlorosilane self-assembled monolayer aluminum-induced crystallization of amorphous silicon

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Simple nanofabrication of a superhydrophobic and transparent biomimetic surface

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Chinese Science Bulletin 2009年第19期54卷 3613-3616页

作者： LIM Hyuneui JUNG Dae-Hwan NOH Jung-Hyun CHOI Gyeong-Rin KIM Wan-Doo Nano-Mechanical Systems Research Division Korea Institute of Machinery and Materials Biotech and nanotech Division Ministry of Knowledge Economy

This paper describes a simple fabrication method for creating superhydrophobic and transparent glass surfaces that mimic natural surfaces such as lotus leaves, moth eyes or cicada wings. Nanostructured glass surfaces were created by a combination of colloidal lithography and plasma etching. A colloidal mask was formed simply by the spin coating of the polystyrene beads and with modification of the interparticle distance between the beads. The etching of the glasses was conducted by CF4 plasma. Tower-shaped nanostructures at an aspect ratio of 1:4 were treated using fluoroalkylsilane selfassembled monolayers (SAMs) to obtain the hydrophobic surfaces. The treated glass surfaces showed superhydrophobicity with a water contact angle of around 150° and a hexadecane contact angle of around 110°. Furthermore, the nanostructured glass was transparent to visible light.

关键词： 21世纪实验室进展聚苯乙烯

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On-surface activation of benzylic C-H bonds for the synthesis of pentagon-fused graphene nanoribbons

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Nano Research 2021年第12期14卷 4754-4759页

作者： Xiushang Xu Marco Di Giovannantonio José I.Urgel Carlo A.Pignedoli Pascal Ruffieux Klaus Müllen Roman Fasel Akimitsu Narita Present address:Istituto di Struttura della Materia-CNR(ISM-CNR) via Fosso del Cavaliere 10000133RomaItaly Present address:IMDEA Nanoscience C/Faraday 9Campus de Cantoblanco28049MadridSpain Max Planck Institute for Polymer Research 55128MainzGermany Empa Swiss Federal Laboratories for Materials Science and Technologynanotech@surfaces Laboratory8600DübendorfSwitzerland Organic and Carbon Nanomaterials Unit Okinawa Institute of Science and Technology Graduate University1919-1 TanchaOnna-sonKunigami-gunOkinawa904-0495Japan Institute of Physical Chemistry Johannes Gutenberg University MainzDuesbergweg 10-1455128MainzGermany

Graphene nanoribbons (GNRs) have potential for applications in electronic devices. A key issue, thereby, is the fine-tuning of their electronic characteristics, which can be achieved through subtle structural modifications. These are not limited to the conventional armchair, zigzag, and cove edges, but also possible through incorporation of non-hexagonal rings. On-surface synthesis enables the fabrication and visualization of GNRs with atomically precise chemical structures, but strategies for the incorporation of non-hexagonal rings have been underexplored. Herein, we describe the on-surface synthesis of armchair-edged GNRs with incorporated five-membered rings through the C-H activation and cyclization of benzylic methyl groups. Ortho-Tolyl-substituted dibromobianthryl was employed as the precursor monomer, and visualization of the resulting structures after annealing at 300 °C on a gold surface by high-resolution noncontact atomic force microscopy clearly revealed the formation of methylene-bridged pentagons at the GNR edges. These persisted after annealing at 340 °C, along with a few fully conjugated pentagons having singly-hydrogenated apexes. The benzylic methyl groups could also migrate or cleave-off, resulting in defects lacking the five-membered rings. Moreover, unexpected and unique structural rearrangements, including the formation of embedded heptagons, were observed. Despite the coexistence of different reaction pathways that hamper selective synthesis of a uniform structure, our results provide novel insights into on-surface reactions en route to functional, non-benzenoid carbon nanomaterials.

关键词： graphene nanoribbons on-surface synthesis scanning-tunneling microscope noncontact atomic force microscope C-H activation

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On-Surface Synthesis of Anthracene-Fused Zigzag Graphene Nanoribbons from 2,7-Dibromo-9,9′-bianthryl Reveals Unexpected Ring Rearrangements

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Precision Chemistry 2024年第2期2卷 81-87页

作者： Xiushang Xu Amogh Kinikar Marco Di Giovannantonio Carlo A.Pignedoli Pascal Ruffieux Klaus Müllen Roman Fasel Akimitsu Narita Max Planck Institute for Polymer Research 55128 MainzGermany Organic and Carbon Nanomaterials Unit Okinawa Institute of Science and Technology Graduate UniversityKunigami-gunOkinawa 904-0495Japan Empa Swiss Federal Laboratories for Materials Science and Technologynanotech@surfaces Laboratory8600 DübendorfSwitzerland Institute of Structure of Matter-CNR(ISM-CNR) 00133 RomaItaly Institute of Physical Chemistry Johannes Gutenberg University Mainz55128 MainzGermany Department of Chemistry Biochemistry and Pharmaceutical SciencesUniversity of Bern3012 BernSwitzerland

On-surface synthesis has emerged as a powerful strategy to fabricate unprecedented forms of atomically precise graphene nanoribbons(GNRs).However,the on-surface synthesis of zigzag GNRs(ZGNR)has met with only limited ***,we report the synthesis and on-surface reactions of 2,7-dibromo-9,9′-bianthryl as the precursor towardπ-extended *** by scanning tunneling microscopy and high-resolution noncontact atomic force microscopy clearly demonstrated the formation of anthracene-fused *** skeletal rearrangements were also observed,which could be explained by intramolecular Diels-Alder *** calculations of the electronic properties of the anthracene-fused ZGNRs revealed spin-polarized edge-states and a narrow bandgap of 0.20 eV.

关键词： On-surface synthesis Graphene nanoribbon On-surface reaction Rearrangement Edge state

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Dynamic observation of in-plane h-BN/graphene heterostructures growth on Ni(lll)

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Nano Research 2020年第7期13卷 1789-1794页

作者： Wei Wei Jiaqi Pan Chanan Euaruksakul Yang Yang Yi Cui Qiang Fu Xinhe Bao Vacuum Interconnected nanotech Workstation Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China Synchrotron Light Research Institute Nakhon Ratchasima 30000Thailand State Key laboratory of Catalysis iChEMDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Department of Chemical Physics University of Science and Technology of ChinaHefei 230026China

The lateraI incorporation of graphene and hexagonal boron nitride(h-BN)onto a substrate surface creates irvplane h-BN/graphene heterostructures,which have promising applications in novel two-dimensional electronic and photoelectronic *** quality of h-BN/graphene domain boundaries depends on their orientation,which is crucial for device ***,the heteroepitaxial growth of graphene along the edges of h-BN domains on Ni(111)surfaces as well as the growth dynamics of h-BN using chemical vapor deposit!on(CVD)are in situ investigated by surface imaging *** nucieating seed effect of h-BN has been revealed,which con tributes to the single orie ntation of heterostructures with epitaxial stitch i ***,the growth of h-BN prior to that of graphene is essential to obtain high-quality in-plane h-BN/graphene heterostructures on Ni(111).The“compact to fractal”shape transition of h-BN domains appears with the increasing surface concentration of the growth blocks,suggesting that the dynamic growth mechanism follows diffusion-limited aggregation(DLA)but not reaction・limited aggregation(RLA).Our results provide in sights into the syn thesis of well-defi ned h-BN/graphene heterostructures and deep un derstanding of the growth dynamics of h-BN on metal surfaces.

关键词： hexagonal boron nitride(h-BN) graphene irnplane heterostructures growth dynamics

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Large-area growth of ultra-high-density single-walled carbon nanotube arrays on sapphire surface

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Nano Research 2015年第11期8卷 3694-3703页

作者： Lixing Kang Yue Hu Hua Zhong Jia Si Shuchen Zhang Qiuchen Zhao Jingjing Lin Qingwen Li Zhiyong Zhang Lianmao Peng Jin Zhang Division ofAdvanced Nanomaterials Suzhou Institute of Nanotech and Nanobionics Chinese Academy of Sciences Suzhou 215123 China Center for Nanochemistry Beijing Science and Engineering Technology Research Center for Low Dimensional Carbon Materials College of Chemistry and Molecular Engineering Peking University Beijing 100871 China University of ChineseAcademy of Sciences Beijing 100049 China 4 Key Laboratory for the Physics and Chemistry of Nanodevices Department of Electronics Peking University Beijing 100871 China Key laboratory for the Physics and Chemistry of Nanodevices Department of Electronics Peking University Beijing 100871 China

A scalable approach to obtaining high-density, large-area single-walled carbon nanotube （SWNT） arrays is essential for realizing the full potential of SWNTs in practical electronic devices; this is still a great challenge. Here, we report an improved synthetic method for large-area growth of ultra-high-density SWNT arrays on sapphire surfaces by combining Trojan catalysts （released from the substrate, to assure ultra-high density） with Mo nanoparticles （loaded on the surface, to stabilize the released Trojan catalysts） as cooperating catalysts. Dense and perfectly aligned SWNTs covered the entire substrate and the local density was as high as 160 tubes/pro. Field-effect transistors （FETs） built on such arrays gave an output current density of -488 μA/μm at the drain-source voltage （Vds） = the gate-source voltage （Vgs） = -2 V, corresponding to an on-conductance per width of 244 μS/μm. These results confirm the wide range of potential applications of Trojan-Mo catalysts in the structure-controlled growth of SWNTs.

关键词： single-walled carbon nanotube arrays ultra-high density large area cooperating catalysts

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Crystal-plane-dependent redox reaction on Cu surfaces

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Nano Research 2020年第6期13卷 1677-1685页

作者： Yangsheng Li Hao Chen Weijia Wang Wugen Huang Yanxiao Ning Qingfei Liu Yi Cui Yong Han Zhi Liu Fan Yang Xinhe Bao State Key laboratory of Catalysis CAS Center for Excellence in NanoscienceCollaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China University of Chinese Academy of Sciences Beijing100049China School of Physical Science and Technology ShanghaiTech UniversityShanghai201210China Vacuum Interconnected nanotech Workstation Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou215123China State Key laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai200050China

The dynamic redox process of surface oxide layers on metal surfaces is of great significance for understanding the active phase in catalytic *** studied the formation of surface oxide layers on Cu(111)and Cu(110)in O2,as well as the subsequent reduction by CO using in situ scanning tunneling microscopy(STM)and X-ray photoelectron spectroscopy(XPS).By monitoring and comparing the oxidation process of Cu(111)and Cu(110)surfaces,we found a crystal-plane-dependent reaction mechanism,which also applies to the reduction of surface oxide layers on Cu *** found XPS Cu spectra cannot be used to identify the various surface oxide layer on Cu surfaces,suggesting their presence in catalytic reactions might have been *** combination of STM and XPS studies are thus advantageous in identifying surface oxide structures and pinpointing the active phases in the redox process,which paves the way for engineering the catalyst and reaction environment for optimized catalytic performances.

关键词： in situ STM NAP-XPS surface oxide Cu(111) Cu(110)

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Growth,coalescence,and etching of two-dimensional overlayers on metals modulated by near-surface Ar nanobubbles

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Nano Research 2022年第3期15卷 2706-2714页

作者： Wei Wei Jiaqi Pan Haiping Lin Chanan Euaruksakul Zhiyun Li Rong Huang Li Wang Zhujun Wang Qiang Fu Yi Cui Vacuum Interconnected nanotech Workstation Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123China Synchrotron Light Research Institute Nakhon Ratchasima 30000Thailand School of Physical Science and Technology Shanghai Tech UniversityShanghai 200031China Scientific Center for Optical and Electron Microscopy ETH Zürich8093 ZürichSwitzerland State Key laboratory of Catalysis iChEMDalian Institute of Chemical Physicsthe Chinese Academy of SciencesDalian 116023China

The synthesis of high-quality ultrathin overlayers is critically dependent on the surface structure of substrates,especially involving the overlayer–substrate *** using in situ surface measurements,we demonstrate that the overlayer–substrate interaction can be tuned by doping near-surface Ar *** interfacial coupling strength significantly decreases with near-surface Ar nanobubbles,accompanying by an“anisotropic to isotropic”growth *** the substrate containing near-surface Ar,the growth front crosses entire surface atomic steps in both uphill and downhill directions with no difference,and thus,the morphology of the two-dimensional(2D)overlayer exhibits a ***,the round-shaped 2D overlayers coalesce seamlessly with a growth acceleration in the approaching direction,which is barely observed in the synthesis of 2D *** can be attributed to the immigration lifetime and diffusion rate of growth species,which depends on the overlayer–substrate interaction and the surface ***,the“round to hexagon”morphological transition is achieved by etching-regrowth,revealing the inherent growth kinetics under quasi-freestanding *** findings provide a novel promising way to modulate the growth,coalescence,and etching dynamics of 2D materials on solid surfaces by adjusting the strength of overlayer–substrate interaction,which contributes to optimization of large-scale production of 2D material crystals.

关键词： two dimensional materials overlayer–substrate interaction near-surface Ar nanobubbles evolution behavior surface dynamics

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Common workflows for computing material properties using different quantum engines

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npj Computational Materials 2021年第1期7卷 1202-1213页

作者： Sebastiaan P.Huber Emanuele Bosoni Marnik Bercx Jens Bröder Augustin Degomme Vladimir Dikan Kristjan Eimre Espen Flage-Larsen Alberto Garcia Luigi Genovese Dominik Gresch Conrad Johnston Guido Petretto Samuel Poncé Gian-Marco Rignanese Christopher J.Sewell Berend Smit Vasily Tseplyaev Martin Uhrin Daniel Wortmann Aliaksandr V.Yakutovich Austin Zadoks Pezhman Zarabadi-Poor Bonan Zhu Nicola Marzari Giovanni Pizzi Theory and Simulation of Materials(THEOS)and National Centre for Computational Design and Discovery of Novel Materials(MARVEL) École Polytechnique Fédérale de LausanneLausanneSwitzerland Institut de Ciència de Materials de Barcelona ICMAB-CSICBellaterraSpain Peter Grünberg Institut and Institute for Advanced Simulation Forschungszentrum JülichJülichGermany Department of Physics RWTH Aachen UniversityAachenGermany CEA IRIG-MEM-L_SimUniv.Grenoble-AlpesGrenobleFrance nanotech@surfaces laboratory Swiss Federal Laboratories for Materials Science and Technology(Empa)DübendorfSwitzerland SINTEF Industry Materials PhysicsOsloNorway Department of Physics University of OsloOsloNorway Microsoft Station Q University of CaliforniaSanta BarbaraCAUSA Atomistic Simulation Centre School of Mathematics and PhysicsQueen’s University BelfastBelfastUK UCLouvain Institut de la Matière Condensée et des Nanosciences(IMCN)Louvain-la-NeuveBelgium laboratory of Molecular Simulation(LSMO) Institut des sciences et ingénierie chimiques(ISIC)École Polytechnique Fédérale de Lausanne(EPFL)ValaisSionSwitzerland Department of Chemistry Claverton DownUniversity of BathBathUK The Faraday Institution DidcotUK Department of Chemistry University College LondonLondonUK

The prediction of material properties based on density-functional theory has become routinely common,thanks,in part,to the steady increase in the number and robustness of available simulation *** plurality of codes and methods is both a boon and a *** providing great opportunities for cross-verification,these packages adopt different methods,algorithms,and paradigms,making it challenging to choose,master,and efficiently use *** demonstrate how developing common interfaces for workflows that automatically compute material properties greatly simplifies interoperability and *** introduce design rules for reusable,code-agnostic,workflow interfaces to compute well-defined material properties,which we implement for eleven quantum engines and use to compute various material *** implementation encodes carefully selected simulation parameters and workflow logic,making the implementer’s expertise of the quantum engine directly available to *** workflows are made available as open-source and full reproducibility of the workflows is guaranteed through the use of the AiiDA infrastructure.

关键词： quantum routine material

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