Journal Article

PUBDB-2024-05033

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Understanding the role of supported Rh atoms and clusters during hydroformylation and CO hydrogenation reactions with in situ / operando XAS and DRIFT spectroscopy

Sarma, B. B. (Corresponding author)Extern* ; Neukum, D.Extern* ; Doronkin, D.Extern* ; Lakshmi Nilayam, A. R. ; Baumgarten, L.Extern* ; Krause, B.Extern* ; Grunwaldt, J.-D.Extern*

2024
RSC Cambridge

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Please use a persistent id in citations: doi:10.1039/D4SC02907K  doi:10.3204/PUBDB-2024-05033

Abstract: Supported Rh single-atoms and clusters on CeO2, MgO, and ZrO2 were investigated as catalysts for hydroformylation of ethylene to propionaldehyde and CO hydrogenation to methanol/ethanol with in situ/operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and X-ray absorption spectroscopy (XAS). Under hydroformylation reaction conditions, operando spectroscopic investigations unravel the presence of both single atoms and clusters and detected at first propanal and then methanol. We find that the formation of methanol is associated with CO hydrogenation over Rh clusters which was further confirmed under CO hydrogenation conditions at elevated pressure. The activity of catalysts synthesized via a precipitation (PP) method over various supports towards the hydroformylation reaction follows the order: Rh/ZrO2 > Rh/CeO2 > Rh/MgO. Comparing Rh/CeO2 catalysts synthesized via different methods, catalysts prepared by flame spray pyrolysis (FSP) showed catalytic activity for the hydroformylation reaction at lower temperatures (413 K), whereas catalysts prepared by wet impregnation (WI) showed the highest stability. These results not only provide fundamental insights into the atomistic level of industrially relevant reactions but also pave the way for a rational design of new catalysts in the future.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
2. FS-Proposal: I-20200891 (I-20200891) (I-20200891)
3. FS-Proposal: I-20211473 (I-20211473) (I-20211473)
4. SFB 1441 B03 - In situ/operando-Charakterisierung von Edelmetallclustern und Partikeln auf Metalloxiden unter Reaktionsbedingungen (B03) (446701131) (446701131)

Experiment(s):

1. PETRA Beamline P65 (PETRA III)

Appears in the scientific report 2024

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Database coverage:
; ; ; ; Chemical Reactions ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; DOAJ Seal ; Essential Science Indicators ; IF >= 5 ; Index Chemicus ; JCR ; National-Konsortium ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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