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


Ontology type: schema:ScholarlyArticle      Open Access: True


Article Info

DATE

2021-06-22

AUTHORS

Jacob Johny, Oleg Prymak, Marius Kamp, Florent Calvo, Se-Ho Kim, Anna Tymoczko, Ayman El-Zoka, Christoph Rehbock, Ulrich Schürmann, Baptiste Gault, Lorenz Kienle, Stephan Barcikowski

ABSTRACT

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 counterparts. Most of their properties strongly depend on their chemical composition, crystallographic structure, and phase distribution. However, 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 catalysis. Au-Fe is a promising bimetallic system where the low-cost and magnetic Fe is combined with catalytically active and plasmonic Au. Here, we report on the in situ temporal evolution of the crystalline ordering in Au-Fe nanoparticles, obtained from a modern laser ablation in liquids synthesis. Our 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 resolution. We show that the Au-Fe nanoparticles initially exhibit highly complex internal nested nanostructures with a wide range of compositions, phase distributions, and size-depended microstrains. The 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 structures. Uncovering 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 conditions. Furthermore, the in situ evaluation of the crystal structure changes upon heating is potentially relevant for high-temperature process utilization of bimetallic nanoparticles, e.g., during catalysis. More... »

PAGES

581-592

Identifiers

URI

http://scigraph.springernature.com/pub.10.1007/s12274-021-3524-7

DOI

http://dx.doi.org/10.1007/s12274-021-3524-7

DIMENSIONS

https://app.dimensions.ai/details/publication/pub.1139064620


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23 schema:description 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 counterparts. Most of their properties strongly depend on their chemical composition, crystallographic structure, and phase distribution. However, 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 catalysis. Au-Fe is a promising bimetallic system where the low-cost and magnetic Fe is combined with catalytically active and plasmonic Au. Here, we report on the in situ temporal evolution of the crystalline ordering in Au-Fe nanoparticles, obtained from a modern laser ablation in liquids synthesis. Our 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 resolution. We show that the Au-Fe nanoparticles initially exhibit highly complex internal nested nanostructures with a wide range of compositions, phase distributions, and size-depended microstrains. The 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 structures. Uncovering 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 conditions. Furthermore, the in situ evaluation of the crystal structure changes upon heating is potentially relevant for high-temperature process utilization of bimetallic nanoparticles, e.g., during catalysis.
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29 schema:keywords Au
30 Au-Fe
31 Au-Fe nanoalloys
32 Au-Fe nanoparticles
33 Fe
34 X-ray diffraction
35 ablation
36 analysis
37 applications
38 atom probe tomography
39 atom resolution
40 atomistic simulations
41 bimetallic nanoparticles
42 bimetallic systems
43 biomedical applications
44 body-centered cubic phase
45 candidates
46 cases nanoparticles
47 catalysis
48 changes
49 characterization
50 chemical composition
51 composition
52 conditions
53 contact
54 counterparts
55 crystal structure
56 crystal structure changes
57 crystalline ordering
58 crystallographic structure
59 cubic phase
60 depth analysis
61 detailed structural characterization
62 diffraction
63 distribution
64 electron microscopy
65 elemental distribution
66 elevated temperatures
67 equilibrium
68 evaluation
69 evolution
70 features
71 formation
72 formation mechanism
73 fundamental viewpoint
74 further insight
75 heating
76 high-temperature catalysis
77 insights
78 knowledge
79 laser ablation
80 liquid synthesis
81 magnetic Fe
82 magnetic properties
83 mechanism
84 metastability
85 microscopy
86 microstrain
87 monometallic counterparts
88 multidimensional
89 nanoalloys
90 nanoparticle formation mechanism
91 nanoparticles
92 nanoscale
93 nanostructures
94 non-equilibrium conditions
95 ordering
96 phase
97 phase distribution
98 plasmonic Au
99 probe tomography
100 process utilization
101 properties
102 range
103 recrystallization
104 resolution
105 simulations
106 single-atom resolution
107 situ evaluation
108 structural characterization
109 structure
110 structure changes
111 superior candidate
112 synthesis
113 system
114 temperature
115 temporal evolution
116 time
117 tomography
118 transformation
119 transmission electron microscopy
120 ultrastructure
121 unique nanostructure
122 utilization
123 viewpoint
124 wide range
125 schema:name Multidimensional thermally-induced transformation of nest-structured complex Au-Fe nanoalloys towards equilibrium
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