Pittkowski, Rebecca K; Clausen, Christian M; Chen, Qinyi; Stoian, Dragos; van Beek, Wouter; Bucher, Jan; Welten, Rahel L; Schlegel, Nicolas; Mathiesen, Jette K; Nielsen, Tobias M; Du, Jia; Rosenkranz, Asger W; Bøjesen, Espen D; Rossmeisl, Jan; Jensen, Kirsten M Ø; Arenz, Matthias (2023). The more the better: on the formation of single-phase high entropy alloy nanoparticles as catalysts for the oxygen reduction reaction. EES catalysis, 1(6), pp. 950-960. Royal Society of Chemistry 10.1039/d3ey00201b
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High entropy alloys (HEAs) are an important new material class with significant application potential in catalysis and electrocatalysis. The entropy-driven formation of HEA materials requires high temperatures and controlled cooling rates. However, catalysts in general also require highly dispersed materials, i.e., nanoparticles. Only then a favorable utilization of the expensive raw materials can be achieved. Several recently reported HEA nanoparticle synthesis strategies, therefore, avoid the high-temperature regime to prevent particle growth. In our work, we investigate a system of five noble metal single-source precursors with superior catalytic activity for the oxygen reduction reaction. Combining in situ X-ray powder diffraction with multi-edge X-ray absorption spectroscopy, we address the fundamental question of how single-phase HEA nanoparticles can form at low temperatures. It is demonstrated that the formation of HEA nanoparticles is governed by stochastic principles and the inhibition of precursor mobility during the formation process favors the formation of a single phase. The proposed formation principle is supported by simulations of the nanoparticle formation in a randomized process, rationalizing the experimentally found differences between two-element and multi-element metal precursor mixtures.
Item Type: |
Journal Article (Original Article) |
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Division/Institute: |
08 Faculty of Science > Department of Chemistry, Biochemistry and Pharmaceutical Sciences (DCBP) |
UniBE Contributor: |
Bucher, Jan Rudolf, Welten, Rahel Lea, Schlegel, Nicolas, Du, Jia, Arenz, Matthias |
Subjects: |
500 Science > 570 Life sciences; biology 500 Science > 540 Chemistry |
ISSN: |
2753-801X |
Publisher: |
Royal Society of Chemistry |
Language: |
English |
Submitter: |
Pubmed Import |
Date Deposited: |
29 Nov 2023 11:04 |
Last Modified: |
29 Nov 2023 11:14 |
Publisher DOI: |
10.1039/d3ey00201b |
PubMed ID: |
38013789 |
BORIS DOI: |
10.48350/189517 |
URI: |
https://boris.unibe.ch/id/eprint/189517 |
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