In:
Physical Chemistry Chemical Physics, Royal Society of Chemistry (RSC), Vol. 23, No. 47 ( 2021), p. 26661-26673
Kurzfassung:
To understand elementary reaction steps in the hydrogenation of CO 2 over copper-based catalysts, we experimentally study the adsorption of CO 2 and H 2 onto cationic Cu n + clusters. For this, we react Cu n + clusters formed by laser ablation with a mixture of H 2 and CO 2 in a flow tube-type reaction channel and characterize the products formed by IR multiple-photon dissociation spectroscopy employing the IR free-electron laser FELICE. We analyze the spectra by comparing them to literature spectra of Cu n + clusters reacted with H 2 and with new spectra of Cu n + clusters reacted with CO 2 . The latter indicate that CO 2 is physisorbed in an end-on configuration when reacted with the clusters alone. Although the spectra for the co-adsorption products evidence H 2 dissociation, no signs for CO 2 activation or reduction are observed. This lack of reactivity for CO 2 is rationalized by density functional theory calculations, which indicate that CO 2 dissociation is hindered by a large reaction barrier. CO 2 reduction to formate should energetically be possible, but the lack of formate observation is attributed to kinetic hindering.
Materialart:
Online-Ressource
ISSN:
1463-9076
,
1463-9084
Sprache:
Englisch
Verlag:
Royal Society of Chemistry (RSC)
Publikationsdatum:
2021
ZDB Id:
1476283-3
ZDB Id:
1476244-4
ZDB Id:
1460656-2
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