How the crystal structure and phase segregation of Au–Fe alloy nanoparticles are ruled by the molar fraction and size

Tymoczko, Anna; Kamp, Marius; Prymak, Oleg; Rehbock, Christoph; Jakobi, Jurij; Schürmann, Ulrich; Kienle, Lorenz; Barcikowski, Stephan

doi:10.1039/c8nr03962c

Cited by 52 publications

(79 citation statements)

References 18 publications

(19 reference statements)

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“…[202] In a recent study, the thermodynamic model also has been experimentally proven to precisely predict FeÀ Au core-shell segregation gained from LAL of a FeÀ Au molar fraction series. [203] Interestingly, the predictions based on simple thermodynamic calculations of free surface energies fit surprisingly well with the experimental observations, [263] although neither solvent contribution to surface energy nor kinetic aspects were being considered in the model. Obviously, thermodynamically-allowed species are formed to a larger extent even under the instantly ultrafast dynamics of nanoparticle formation during LAL.…”

Section: Composition and Morphology Controlmentioning

confidence: 64%

“…Driven by thermodynamically‐favored interfacial and surface energies between elemental Ag and Cu, the segregation tendency of NP with different size and composition can be predicted . In a recent study, the thermodynamic model also has been experimentally proven to precisely predict Fe−Au core‐shell segregation gained from LAL of a Fe−Au molar fraction series . Interestingly, the predictions based on simple thermodynamic calculations of free surface energies fit surprisingly well with the experimental observations, although neither solvent contribution to surface energy nor kinetic aspects were being considered in the model.…”

Section: Laser‐based Materials Design: Multi‐elemental Nanoparticlesmentioning

confidence: 92%

“…Interestingly, the predictions based on simple thermodynamic calculations of free surface energies fit surprisingly well with the experimental observations, although neither solvent contribution to surface energy nor kinetic aspects were being considered in the model. Obviously, thermodynamically‐allowed species are formed to a larger extent even under the instantly ultrafast dynamics of nanoparticle formation during LAL . In fact, by particle analysis during in situ TEM heating experiments, Kamp et.…”

Section: Laser‐based Materials Design: Multi‐elemental Nanoparticlesmentioning

confidence: 99%

“…Despite the given examples, the catalytic activity of laser‐generated nanoalloys has only scarcely been targeted and rarely been compared to chemically synthesized analogs in present literature, yet. It may be noted, that due to the high‐temperature gradients during laser‐based nanoparticle synthesis (compare section 3.2), the formation of multielement‐nanoparticles is kinetically controlled to some degree, allowing the formation of meta‐stable phases above thermodynamic minimum or room temperature species expected from the phase diagram, respectively . In turn, wet‐chemical processes rather follow thermodynamics eventually leading to elemental gradients within prepared multi‐elemental nanoparticles compared to laser‐generated analogous .…”

Section: Laser‐based Materials Design: Multi‐elemental Nanoparticlesmentioning

confidence: 99%

“…Obviously, thermodynamically-allowed species are formed to a larger extent even under the instantly ultrafast dynamics of nanoparticle formation during LAL. [203] In fact, by particle analysis during in situ TEM heating experiments, Kamp et. al.…”

Section: Composition and Morphology Controlmentioning

confidence: 99%

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Perspective of Surfactant‐Free Colloidal Nanoparticles in Heterogeneous Catalysis

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Due to material gaps and synthesis‐related cross‐correlations in heterogeneous catalysis, chemists and physicists are constantly motivated to develop novel catalyst preparation methods for independent control of morphology, size, and composition. Within this article, advances, opportunities, and the current limits of laser‐based catalyst preparation technique, as well as synergies with conventional methods will be reviewed in terms of purity, particle size, morphology, composition, and nanoparticle‐support interaction. It will be shown, that the surfactant‐free particles represent ideal model materials to validate kinetic models and conduct parametric activity studies by independent adjustment of functional properties like nanoparticle size, composition, and load. Consequently, the importance of transient plasma dynamics tailoring nanoparticle formation will be pointed out, comparing experimental studies with own calculations and novel simulations taken from literature. Finally, perspectives of surfactant‐free colloidal nanoparticles for unrevealing active sites in heterogeneous catalysts are presented.

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Section: Composition and Morphology Controlmentioning

confidence: 64%

Section: Laser‐based Materials Design: Multi‐elemental Nanoparticlesmentioning

confidence: 92%

Section: Laser‐based Materials Design: Multi‐elemental Nanoparticlesmentioning

confidence: 99%

Section: Laser‐based Materials Design: Multi‐elemental Nanoparticlesmentioning

confidence: 99%

Section: Composition and Morphology Controlmentioning

confidence: 99%

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Perspective of Surfactant‐Free Colloidal Nanoparticles in Heterogeneous Catalysis

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Room‐Temperature Laser Synthesis in Liquid of Oxide, Metal‐Oxide Core‐Shells, and Doped Oxide Nanoparticles

Amendola

Amans

Ishikawa

et al. 2020

Chemistry A European J

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211

179

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Although oxide nanoparticles are ubiquitous in science and technology, a multitude of compositions, phases, structures, and doping levels exist, each one requiring a variety of conditions for their synthesis and modification. Besides, experimental procedures are frequently dominated by high temperatures or pressures and by chemical contaminants or waste. In recent years, laser synthesis of colloids emerged as a versatile approach to access a library of clean oxide nanoparticles relying on only four main strategies running at room temperature and ambient pressure: laser ablation in liquid, laser fragmentation in liquid, laser melting in liquid and laser defect‐engineering in liquid. Here, established laser‐based methodologies are reviewed through the presentation of a panorama of oxide nanoparticles which include pure oxidic phases, as well as unconventional structures like defective or doped oxides, non‐equilibrium compounds, metal‐oxide core–shells and other anisotropic morphologies. So far, these materials showed several useful properties that are discussed with special emphasis on catalytic, biomedical and optical application. Yet, given the endless number of mixed compounds accessible by the laser‐assisted methodologies, there is still a lot of room to expand the library of nano‐crystals and to refine the control over products as well as to improve the understanding of the whole process of nanoparticle formation. To that end, this review aims to identify the perspectives and unique opportunities of laser‐based synthesis and processing of colloids for future studies of oxide nanomaterial‐oriented sciences.

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Synthesis of High Entropy Alloy Nanoparticles by Pulsed Laser Ablation in Liquids: Influence of Target Preparation on Stoichiometry and Productivity

Tahir,

Shkodich,

Eggert

et al. 2024

ChemNanoMat

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High entropy alloys (HEAs) have a wide range of applications across various fields, including structural engineering, biomedical science, catalysis, magnetism, and nuclear technology. Nanoscale HEA particles show promising catalytic properties. Nevertheless, attaining versatile composition control in nanoparticles poses a persistent challenge. This study proposes the use of pulsed laser ablation in liquids (PLAL) for synthesizing nanoparticles using equiatomic CoCrFeMnNi targets with varied preparation methods. We evaluate the impact of target preparation method on nanoparticle yield and composition as well as the magnetic properties of the nanoparticles. The elemental powder‐pressed heat‐treated target (HEA‐PP), identified as the most time‐efficient and cost‐effective, exhibits noticeable segregation and non‐uniform elemental distribution compared to ball milled hot‐pressed powder (HEA‐BP) and face‐centered cubic (FCC) single crystal (HEA‐SX) alloy targets. From all targets, nanoparticles (sizes from 2 to 120 nm) can be produced in ethanol with a nearly equiatomic CoCrFeMnNi composition and a FCC structure, showing oxidation of up to 20 at.%. Nanoparticles from HEA‐PP exist in a solid solution state, while those from HEA‐BP and HEA‐SX form core‐shell structures with a Mn shell due to inhomogeneous material expulsion, confirmed by mass spectrometry. HEA‐PP PLAL synthesis demonstrates 6.8 % and 15.1 % higher productivity compared to HEA‐BP and HEA‐SX, establishing PLAL of elemental powder‐pressed targets as a reliable, time‐efficient, and cost‐effective method for generating solid solution HEA nanoparticles.

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How the crystal structure and phase segregation of Au–Fe alloy nanoparticles are ruled by the molar fraction and size

Cited by 52 publications

References 18 publications

Perspective of Surfactant‐Free Colloidal Nanoparticles in Heterogeneous Catalysis

Perspective of Surfactant‐Free Colloidal Nanoparticles in Heterogeneous Catalysis

Room‐Temperature Laser Synthesis in Liquid of Oxide, Metal‐Oxide Core‐Shells, and Doped Oxide Nanoparticles

Synthesis of High Entropy Alloy Nanoparticles by Pulsed Laser Ablation in Liquids: Influence of Target Preparation on Stoichiometry and Productivity

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