Breaking with the Principles of Coreduction to Form Stoichiometric Intermetallic PdCu Nanoparticles

Jette K. Mathiesen, Espen D. Bøjesen*, Jack K. Pedersen, Emil T.S. Kjær, Mikkel Juelsholt, Susan Cooper, Jonathan Quinson, Andy S. Anker, Geoff Cutts, Dean S. Keeble, Maria S. Thomsen, Jan Rossmeisl, Kirsten M.Ø. Jensen*

*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaperJournal articleResearchpeer-review

24 Downloads (Pure)

Abstract

Intermetallic nanoparticles (NPs) have shown enhanced catalytic properties as compared to their disordered alloy counterparts. To advance their use in green energy, it is crucial to understand what controls the formation of intermetallic NPs over alloy structures. By carefully selecting the additives used in NP synthesis, it is here shown that monodisperse, intermetallic PdCu NPs can be synthesized in a controllable manner. Introducing the additives iron(III) chloride and ascorbic acid, both morphological and structural control can be achieved. Combined, these additives provide a synergetic effect resulting in precursor reduction and defect-free growth; ultimately leading to monodisperse, single-crystalline, intermetallic PdCu NPs. Using in situ X-ray total scattering, a hitherto unknown transformation pathway is reported that diverges from the commonly reported coreduction disorder–order transformation. A Cu-rich structure initially forms, which upon the incorporation of Pd(0) and atomic ordering forms intermetallic PdCu NPs. These findings underpin that formation of stoichiometric intermetallic NPs is not limited by standard reduction potential matching and coreduction mechanisms, but is instead driven by changes in the local chemistry. Ultimately, using the local chemistry as a handle to tune the NP structure might open new opportunities to expand the library of intermetallic NPs by exploiting synthesis by design.

Original languageEnglish
Article number2200420
JournalSmall Methods
Volume6
Issue6
Number of pages11
DOIs
Publication statusPublished - Jun 2022

Keywords

  • formation mechanism
  • in situ X-ray total scattering
  • intermetallic nanoparticles
  • synthesis by design

Fingerprint

Dive into the research topics of 'Breaking with the Principles of Coreduction to Form Stoichiometric Intermetallic PdCu Nanoparticles'. Together they form a unique fingerprint.

Cite this