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Laser-generated high entropy metallic glass nanoparticles as bifunctional electrocatalysts

Nano Research 2022年第6期15卷 4807-4819页

作者： Jacob Johny Yao Li Marius Kamp Oleg Prymak Shun-Xing Liang Tobias Krekeler Martin Ritter lorenz kienle Christoph Rehbock Stephan Barcikowski Sven Reichenberger Technical Chemistry I and Center for Nanointegration Duisburg-Essen(CENIDE) University of Duisburg-EssenEssen 45141Germany Institute for Materials Science Synthesis and Real StructureKiel UniversityKiel 24143Germany Inorganic Chemistry and Center for Nanointegration Duisburg-Essen(CENIDE) University of Duisburg-EssenEssen 45141Germany Electron Microscopy Unit Hamburg University of TechnologyHamburg 21073Germany

High entropy metallic glass nanoparticles(HEMG NPs)are very promising materials for energy conversion due to the wide tuning possibilities of electrochemical potentials offered by their multimetallic character combined with an amorphous *** until now,the generation of these HEMG NPs involved tedious synthesis procedures where the generated particles were only available on highly specialized supports,which limited their widespread ***,more flexible synthetic approaches to obtain colloidal HEMG NPs for applications in energy conversion and storage are highly *** utilized pulsed laser ablation of bulk high entropy alloy targets in acetonitrile to generate colloidal carbon-coated CrCoFeNiMn and CrCoFeNiMnMo HEMG *** in-depth analysis of the structure and elemental distribution of the obtained nanoparticles down to single-particle levels using advanced transmission electron microscopy(TEM),energy-dispersive X-ray spectroscopy(EDX),X-ray diffraction(XRD),and Xray photoelectron spectroscopy(XPS)methods revealed amorphous quinary and senary alloy phases with slight manganese oxide/hydroxide surface segregation,which were stabilized within graphitic *** on the catalytic activity of the corresponding carbon-HEMG NPs during oxygen evolution and oxygen reduction reactions revealed an elevated activity upon the incorporation of moderate amounts of Mo into the amorphous alloy,probably due to the defect generation by atomic size ***,we demonstrate the superiority of these carbon-HEMG NPs over their crystalline analogies and highlight the suitability of these amorphous multi-elemental NPs in electrocatalytic energy conversion.

关键词： high entropy alloy pulsed laser ablation in liquid amorphous catalysis oxygen evolution reaction oxygen reduction reaction

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Multidimensional thermally-induced transformation of nest-structured complex Au-Fe nanoalloys towards equilibrium

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Nano Research 2022年第1期15卷 581-592页

作者： Jacob Johny Oleg Prymak Marius Kamp Florent Calvo Se-Ho Kim Anna Tymoczko Ayman El-Zoka Christoph Rehbock Ulrich Schurmann Baptiste Gault lorenz kienle Stephan Barcikowski Technical Chemistry I and Center for Nanointegration Duisburg-Essen(CENIDE) University of Duisburg-EssenEssen 45141Germany Inorganic Chemistry and Center for Nanointegration Duisburg-Essen(CENIDE) University of Duisburg-EssenEssen 45141Germany Institute for Materials Science Synthesis and Real StructureKiel UniversityKiel 24143Germany University Grenoble Alpes CNRSLiPhyGrenoble 38000France Max-Planck-Institut fur Eisenforschurtg GmbH Diisseldorf40237Germany Department of Materials Royal School of MineImperial College LondonLondon SW72AZUK

Bimetallic nanoparticles are often superior candidates for a wide range of technological and biomedical applications owing to their enhanced catalytic,optical,and magnetic properties,which are often better than their monometallic *** of their properties strongly depend on their chemical composition,crystallographic structure,and phase ***,little is known of how their crystal structure,on the nanoscale,transforms over time at elevated temperatures,even though this knowledge is highly relevant in case nanoparticles are used in,e.g.,high-temperature ***-Fe is a promising bimetallic system where the low-cost and magnetic Fe is combined with catalytically active and plasmonic ***,we report on the in s/fi;temporal evolution of the crystalline ordering in Au-Fe nanoparticles,obtained from a modern laser ablation in liquids *** in-depth analysis,complemented by dedicated atomistic simulations,includes a detailed structural characterization by X-ray diffraction and transmission electron microscopy as well as atom probe tomography to reveal elemental distributions down to a single atom *** show that the Au-Fe nanoparticles initially exhibit highly complex internal nested nanostructures with a wide range of compositions,phase distributions,and size-depended *** elevated temperature induces a diffusion-controlled recrystallization and phase merging,resulting in the formation of a single face-centered-cubic ultrastructure in contact with a body-centered cubic phase,which demonstrates the metastability of these *** these unique nanostructures with nested features could be highly attractive from a fundamental viewpoint as they could give further insights into the nanoparticle formation mechanism under non-equilibrium ***,the in situ evaluation of the crystal structure changes upon heating is potentially relevant for high-temperature process utilization of bimetallic na

关键词： nanoparticles in situ atom probe tomography diffusion recrystallization atomistic simulation

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