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Reversible hydrogenation restores defected graphene to graphene

Science China Chemistry 2021年第6期64卷 1047-1056页

作者： Lin Jiang Pauline MGvan Deursen Hadi Arjmandi-Tash Liubov ABelyaeva Haoyuan Qi Jiao He Vincent Kofman Longfei Wu Valery Muravev Ute Kaiser Harold Linnartz emiel jmhensen Jan PHofmann Grégory FSchneider Leiden Institute of Chemistry Leiden UniversityEinsteinweg 552333CC LeidenThe Netherlands Central Facility for Electron Microscopy Electron Microscopy Group of Materials ScienceUlm UniversityAlbert-Einstein-Allee 11Ulm 89081Germany Laboratory for Astrophysics Leiden ObservatoryLeiden UniversityNiels Bohrweg 22333 CA LeidenThe Netherlands Laboratory for Inorganic Materials and Catalysis Department of Chemical Engineering and ChemistryEindhoven University of TechnologyP.O.Box 5135600 MB EindhovenThe Netherlands Center for Advancing Electronics Dresden(cfaed)and Faculty of Chemistry and Food Chemistry Technical University of Dresden010069 DresdenGermany

Graphene as a two-dimensional material is prone to hydrocarbon contaminations,which can significantly alter its intrinsic electrical ***,we implement a facile hydrogenation-dehydrogenation strategy to remove hydrocarbon contaminations and preserve the excellent transport properties of monolayer *** electron microscopy we quantitatively characterized the improved cleanness of hydrogenated graphene compared to untreated *** situ spectroscopic investigations revealed that the hydrogenation treatment promoted the adsorption of water at the graphene surface,resulting in a protective layer against the re-deposition of hydrocarbon ***,the further dehydrogenation of hydrogenated graphene rendered a more pristine-like basal plane with improved carrier mobility compared to untreated pristine *** findings provide a practical post-growth cleaning protocol for graphene with maintained surface cleanness and lattice integrity to systematically carry a range of surface chemistry in the form of a well-performing and reproducible transistor.

关键词： graphene reversible hydrogenation surface cleanness in situ spectroscopy transistors

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Combining video and GPS-tracking to study the spatial foraging distribution of a single-prey loading seabird

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Avian Research 2024年第3期15卷 316-325页

作者： Ruben C.Fijn Wouter Courtens Bas W.R.Engels emiel E.van Loon Judy Shamoun-Baranes Waardenburg Ecology Deparonent of Bird EcologyCulemborgthe Netherlands University of Amsterdam Insnitute for Biodiversity and Ecoasystem DymaomicsAmsterdamthe Netherlands Research Insitute for Nature and Forest(INBO) BrusselsBcgium

Seabirds are valuable indicators of marine ecosystem processes and studying seabird diets can shed light on natural or human-induced variability in food-web *** single-prey loading seabird species such as terns have the potential to act as visual sentinels of prey availability ***,obtaining diet information from remote bird colonies is often challenging and time *** this pilot study we present a novel approach to combine two established methods to study seabird foraging ecology,providing a powerful and cost-effective tool to study the distribution of prey items available to *** combined GPS tracking data of Sandwich Terns(Thalasseus sandvicensis)with prey-observations from a hide in 2012 and 2013,and from semicontinuously recorded camera footage in *** doing so,we identified 115 approximate catch locations of prey(86 herring/sprat Clupeidae,29 sandeel Ammodytidae).Combining GPS-data and prey observations yielded detailed knowledge on the movements and chick diets of tracked birds as well as the spatial origin and lengths of captured prey *** catch distances of both Clupeidae and Ammodytidae resulted in deliveries of larger prey items and thus higher energy yield per trip,but also a higher energy expenditure per *** discuss the limitations and potential of our methodological approach to study foraging energetics during chick-provisioning of seabirds that carry prey items visible in their beaks.

关键词： Diet Digitalfilm Geo-referencing Non-invasive monitoring Provisioning Sandwich Tern Thalasseus sandvicensis

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Lattice oxygen activation in transition metal doped ceria

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Chinese Journal of Catalysis 2020年第6期41卷 977-984页

作者： Ya-Qiong Su Long Zhang Valery Muravev emiel J.M.Hensen Laboratory of Inorganic Materials&Catalysis Schuit Institute of CatalysisEindhoven University of TechnologyP.O.Box 5135600 MB EindhovenThe Netherlands

Density functional theory calculations were carried out to investigate the influence of doping transition metal(TM) ions into the ceria surface on the activation of surface lattice oxygen atoms. For this purpose, the structure and stability of the most stable(111) surface termination of CeO2 modified by TM ions was determined. Except for Zr and Pt dopants that preserve octahedral oxygen coordination, the TM dopants prefer a square-planar coordination when substituting the surface Ce ions. The surface construction from octahedral to square-planar is facile for all TM dopants, except for Pt(1.14 e V) and Zr(square-planar coordination unstable). Typically, the ionic radius of tetravalent TM cations is much smaller than that of Ce4+, resulting a significant tensile-strained lattice and explaining the lowered oxygen vacancy formation energy. Except for Zr, the square-planar structure is the preferred one when one oxygen vacancy is created. Thermodynamic analysis shows that TM-doped CeO2 surfaces contain oxygen defects under typical conditions of environmental catalysis. A case of practical importance is the facile lattice oxygen activation in Zr-doped CeO2(111), which benefits CO oxidation. The findings emphasize the origin of lattice oxygen activation and the preferred location of TM dopants in TM-ceria solid solution catalysts.

关键词： Lattice oxygen activation TM-doped CeO2(111) Density functional theory calculations Oxygen vacancy Square-planar coordination Coordination transformation CO oxidation

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Mo掺杂CeO_(2)催化剂上甲烷的无氧偶联:表面和气相过程

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Chinese Journal of Catalysis 2023年第6期49卷 68-80页

作者：张昊苏亚琼 Nikolay Kosinov emiel J.M.Hensen 埃因霍温理工大学化学工程与化学系无机材料与催化实验室荷兰埃因霍温西安交通大学化学学院储能材料与设备教育部工程研究中心国家储能技术产教融合创新平台(中心)陕西西安710049

甲烷无氧偶联是一种很有前景的甲烷转化利用的增值途径.由于高温条件下催化剂表面反应与气相自由基反应共存且均对产物分布具有重要影响,因而很难深入理解该反应的机理.本文采用火焰喷雾热解方法制备了一系列具有高度分散Mo位点的Mo掺杂... 详细信息

甲烷无氧偶联是一种很有前景的甲烷转化利用的增值途径.由于高温条件下催化剂表面反应与气相自由基反应共存且均对产物分布具有重要影响,因而很难深入理解该反应的机理.本文采用火焰喷雾热解方法制备了一系列具有高度分散Mo位点的Mo掺杂的CeO_(2)样品,并用于催化甲烷无氧偶联反应.结果表明,在气相产物中,附加值较高的C2烃产物(乙烷和乙烯)的选择性可达98%.反应过程中催化剂中高度分散的Mo-oxo物种被还原并转化为Mo(oxy-)碳化物物种,它是甲烷活化的活性位点.通过改变反应器内气相部分(即无催化剂部分)的体积,研究了气相反应对于产物分布的贡献.乙烷是甲烷无氧偶联的初级产物,部分乙烯和大部分苯是通过气相化学形成的.综上,本文为甲烷无氧偶联高效催化剂的设计提供了参考,并明确了减少反应器中自由体积以限制二次气相反应的重要性.

关键词：甲烷无氧偶联 CeO_(2) Mo 活性位

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用于甲烷芳构化的Mo/HZSM-5催化剂的活化（英文）

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催化学报 2015年第6期36卷 829-837页

作者： Christiaan H.L.Tempelman Xiaochun Zhu emiel J.M.Hensen Laboratory of Inorganic Materials Chemistry Schuit Institute of Catalysis Eindhoven University of Technology

The effect of Mo/HZSM-5 pretreatment at 973 K in inert(He), oxidizing(artificial air), and carburizing(CH4/He mixture) atmospheres on its performance in non-oxidative methane dehydroaromatization(MDA) was investigated. The effect of post-synthesis silylation on deactivation of external acid sites was also studied. Precarburization resulted in increased aromatic selectivity and improved catalyst stability. The benzene selectivity was the highest for the silylated Mo/HZSM-5 catalyst(benzene + naphthalene selectivity after 1 h on stream was close to 100%). The deactivation of precarburized zeolites was less pronounced than that of zeolites heated in air or He. During heating in air or He, larger fractions of the molybdenum oxide species diffused into the micropores than during heating in methane. Carburization of the molybdenum oxide species in the micropores during MDA resulted in the formation of molybdenum carbide particles, and these contributed to pore blocking, making the Brnsted acid sites inaccessible. The formation of molybdenum carbides during heating in methane resulted in a less mobile Mo phase. It is argued that the presence of molybdenum carbide particles in the micropores contributes to rapid catalyst deactivation, in addition to the formation of hard coke on the external surface.

关键词： HZSM-5 甲烷芳构化催化剂失活非氧化性加热过程 MO 激活

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Globalization of Traditional Chinese Medicinal products And New Regulatory Structures in the European Union

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世界科学技术-中医药现代化 2009年第1期11卷 206-213,205页

作者： emiel Van Galen Burt Kroes Medicines Evaluation Board Agency PO BOX 16229 2500 BE The Hague the Netherlands

Traditional Chinese Medicine (TCM) , Registration, EU pharmaceutical legislation, Traditional Herbal Medicinal Products, tHMP, quality, safety, efficacy, traditional use, EMEA, European Medicines Agency, European Phar... 详细信息

关键词：欧洲中医医疗卫生事业发展现状

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Reaching for the brain：stimulating neural activity as the big leap in optic nerve regeneration

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Eye Science 2016年第4期31卷 221-224页

作者： emiel Geeraerts Lieve Moons Lies De Groef Research Group Neural Circuit Development and Regeneration Animal Physiology and Neurobiology Section Department of Biology KU LeuvenLeuven Belgium

In the August issue of Nature Neuroscience,Lim and coworkers reported on their study of axonal regeneration in the adult optic nerve,revealing that combined activation of mammalian target of rapamycin(mTOR)signaling a... 详细信息

关键词：神经再生大脑动作中枢神经系统神经科学视觉中心神经活动 mTOR

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Stability of heterogeneous single-atom catalysts:a scaling law mapping thermodynamics to kinetics

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npj Computational Materials 2020年第1期6卷 460-466页

作者： Ya-Qiong Su Long Zhang Yifan Wang Jin-Xun Liu Valery Muravev Konstantinos Alexopoulos Ivo A.W.Filot Dionisios G.Vlachos emiel J.M.Hensen Laboratory of Inorganic Materials and Catalysis Department of Chemical Engineering and ChemistryEindhoven University of TechnologyP.O.Box 5135600 MB EindhovenThe Netherlands Department of Chemical and Biomolecular Engineering The Delaware Energy InstituteUniversity of Delaware221 Academy St.NewarkDE 19716USA Department of Chemical Engineering University of MichiganAnn ArborMI 48109-2136USA

Heterogeneous single-atom catalysts(SACs)hold the promise of combining high catalytic performance with maximum utilization of often precious *** extend the current thermodynamic view of SAC stability in terms of the binding energy(E_(bind))of singlemetal atoms on a support to a kinetic(transport)one by considering the activation barrier for metal atom diffusion.A rapid computational screening approach allows predicting diffusion barriers for metal-support pairs based on Ebind of a metal atom to the support and the cohesive energy of the bulk metal(E_(c)).

关键词： kinetics thermodynamics scaling

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Particle Size and Crystal Phase Effects in Fischer-Tropsch Catalysts

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Engineering 2017年第4期3卷 467-476页

作者： Jin-xun Liu Peng Wang Wayne Xu emiel J. M. Hensen Laboratory of Inorganic Materials Chemistry Schuit Institute of Catalysis Department of Chemical Engineering and Chemistry Eindhoven University of Technology Eindhoven 5600 MB The Netherlands National Institute of Clean-and-Low-Carhon Energy Beijing 102211 China

Fischer-Tropsch synthesis （FTS） is an increasingly important approach for producing liquid fuels and chemicals via syngas-that is, synthesis gas, a mixture of carbon monoxide and hydrogen-generated from coal, natural gas, or biomass. In FTS, dispersed transition metal nanoparticles are used to catalyze the reactions underlying the formation of carbon-carbon bonds. Catalytic activity and selectivity are strongly correlated with the electronic and geometric structure of the nanoparticles, which depend on the particle size, morphology, and crystallographic phase of the nanoparticles. In this article, we review recent works dealing with the aspects of bulk and surface sensitivity of the FTS reaction. Understanding the different catalytic behavior in more detail as a function of these parameters may guide the design of more active, selective, and stable FTS catalysts.

关键词： Fischer-Tropsch synthesis Iron cobalt and ruthenium carbides Size effect Crystal structure

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Influence of hematite morphology on the CO oxidation performance of Au/α-Fe_(2)O_(3)

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Chinese Journal of Catalysis 2021年第4期42卷 658-665页

作者： Yanan Gao Fu-Kuo Chiang Shaojie Li Long Zhang Peng Wang emiel J.M.Hensen Laboratory of Inorganic Materials and Catalysis Department of Chemical Engineering and ChemistryEindhoven University of TechnologyP.O.Box 5135600 MB EindhovenThe Netherlands National Institute of Clean-and-Low-Carbon Energy Shenhua NICEFuture Science and Technology CityBeijing 102211China

Controlling the interaction between metal nanoparticles and the support is a means to tune catalytic activity and *** we investigated the influence of the morphology of hematite on the performance of gold for CO *** and nanorod forms of hematite,α-Fe_(2)O_(3)(S)andα-Fe_(2)O_(3)(R)respectively,were used to support gold *** surface ofα-Fe_(2)O_(3)(R)was more corrugated than that ofα-Fe_(2)O_(3)(S).These defects provide anchoring sites for gold nanoparticle deposition and *** to the stronger gold-support interactions,Au/α-Fe_(2)O_(3)(R)contained smaller and more hemispherical gold particles than Au/α-Fe_(2)O_(3)(S).Au/α-Fe_(2)O_(3)(R)was not only more active in CO oxidation but also much more stable as evident from the small change in gold particle size during *** higher reducibility of Au/α-Fe_(2)O_(3)(R)also contributed to the higher CO oxidation activity.

关键词： Gold CO oxidation Hematite Morphology Stability

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