Journal Article

PUBDB-2025-01318

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Supported Binuclear Gold Phosphine Complexes as CO Oxidation Catalysts: Insights into the Formation of Surface‐Stabilized Au Particles

Rang, F.Extern* ; Delrieux, T.Extern* ; Maurer, F.Extern* ; Flecken, F. ; Grunwaldt, J.-D.Extern* ; Hanf, S. (Corresponding author)Extern*

2024
Wiley-VCH GmbH Weinheim

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Please use a persistent id in citations: doi:10.1002/smsc.202400345  doi:10.3204/PUBDB-2025-01318

Abstract: Atomically precise gold phosphine complexes as precursors for supported Au catalysts tested in CO oxidation are presented. Using a variety of analytical techniques, including in situ and operando X-ray absorption spectroscopy, it is discovered that minor changes in the ligand of the molecular complexes result in significantly different activation behaviors of supported Au catalysts under reaction conditions. When using [Au$_2$(μ$_2$-POP)$_2$]OTf$_2$ (POP = tetraphenylphosphoxane) as single-source precursor, an active supported oxidation catalyst in second light-off is obtained, outperforming a commercial Au/TiO$_2$ and a P-free Au/Al$_2$O$_3$ reference catalyst. Conversely, using [Au$_2$(μ$_2$-dppe)$_2$]OTf$_2$ (dppe = diphenylphosphinoethane) on alumina leads to a significant decrease in CO oxidation activity. This difference is attributed to the formation of P-containing ligand residues on the support in the case of [Au$_2$(μ$_2$-POP)$_2$]OTf$_2$/Al$_2$O$_3$, which enhances the thermal stability of the Au particles and affects the particle's electronic properties through charge transfer processes. This work provides insights into the dynamic ligand decomposition of molecular gold complexes under reaction conditions and demonstrates the delicate balance between the stabilization of Au particles, clusters, and complexes using ligands and the blocking of active sites. This knowledge will pave the way for the targeted use of molecular transition metal complexes as precursors in synthesizing surface-stabilized nanoparticles.

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Contributing Institute(s):

1. FS DOOR-User (FS DOOR-User)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
2. SFB 1441 C02 - Monolithische Katalysatoren mit enger Partikelgrößenverteilung in Schichten mit definierten Gradienten (C02) (446705995) (446705995)
3. DFG project G:(GEPRIS)460248799 - DAPHNE4NFDI - DAten aus PHoton- und Neutronen Experimenten für NFDI (460248799) (460248799)
4. DFG project G:(GEPRIS)441926934 - NFDI4Cat – NFDI für Wissenschaften mit Bezug zur Katalyse (441926934) (441926934)

Experiment(s):

1. PETRA Beamline P65 (PETRA III)

Appears in the scientific report 2024

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