Sökning: WFRF:(Halldin C)
> Chalmers tekniska högskola >
Acetic acid convers...
Acetic acid conversion to ketene on Cu 2 O(1 0 0): Reaction mechanism deduced from experimental observations and theoretical computations
-
- Tissot, H. (författare)
- Kungliga Tekniska Högskolan (KTH),Royal Institute of Technology (KTH)
-
- Halldin Stenlid, J. (författare)
- Alba Nova Universitetscentrum,AlbaNova University Center. Stockholm Center for Physics, Astronomy and Biotechnology
-
- Wang, C. (författare)
- Kungliga Tekniska Högskolan (KTH),Royal Institute of Technology (KTH)
-
visa fler...
-
- Panahi, M. (författare)
- Koc Universitesi,Koç University
-
- Kaya, S. (författare)
- Koc Universitesi,Koç University
-
- Brinck, T. (författare)
- Kungliga Tekniska Högskolan (KTH),Royal Institute of Technology (KTH)
-
- Sassa, Yasmine, 1981 (författare)
- Chalmers tekniska högskola,Chalmers University of Technology
-
- Johansson, Fredrik O.L. (författare)
- Uppsala universitet,Uppsala University
-
- Weissenrieder, Jonas (författare)
- Kungliga Tekniska Högskolan (KTH),Royal Institute of Technology (KTH)
-
visa färre...
-
(creator_code:org_t)
- Elsevier BV, 2021
- 2021
- Engelska.
-
Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517 .- 1090-2694. ; 402, s. 154-165
- Relaterad länk:
-
https://research.cha... (primary) (free)
-
visa fler...
-
https://doi.org/10.1...
-
https://research.cha...
-
https://doi.org/10.1...
-
visa färre...
Abstract
Ämnesord
Stäng
- Ketene, a versatile reagent in production of fine and specialty chemicals, is produced from acetic acid. We investigate the synthesis of ketene from acetic acid over the (3,0;1,1) surface of Cu2O(1 0 0) through analysis of the adsorption and desorption characteristics of formic and acetic acids. The results allow us to establish a reaction mechanism for ketene formation. Observations from x-ray photoelectron spectroscopy (XPS), scanning tunneling microscopy, and temperature programmed desorption (TPD), supported by a comparison with formic acid results, suggest that acetic acid reacts with Cu2O through deprotonation to form acetate species coordinated to copper sites and hydroxylation of nearby surface oxygen sites. For formic acid the decomposition of adsorbed formate species results in desorption of CO2 and CO while, for acetic acid, high yields of ketene are observed at temperature >500 K. Modeling by density functional theory (DFT) confirms the strong interaction of acetic acid with the (3,0;1,1) surface and the spontaneous dissociation into adsorbed acetate and hydrogen atom species, the latter forming an OH-group. In an identified reaction intermediate ketene binds via all C and O atoms to Cu surface sites, in agreement with interpretations from XPS. In the vicinity of the adsorbate the surface experiences a local reorganization into a c(2 × 2) reconstruction. The total computed energy barrier for ketene formation is 1.81 eV in good agreement with the 1.74 eV obtained from TPD analysis. Our experimental observations and mechanistic DFT studies suggests that Cu2O can operate as an efficient catalyst for the green generation of ketene from acetic acid.
Ämnesord
- NATURVETENSKAP -- Kemi -- Oorganisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)
- NATURVETENSKAP -- Kemi -- Annan kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Other Chemistry Topics (hsv//eng)
- NATURVETENSKAP -- Kemi -- Organisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Organic Chemistry (hsv//eng)
Nyckelord
- Heterogeneous catalysis
- Scanning tunneling microscopy
- Density functional theory
- Ketene
- X-ray photoelectron spectroscopy
- Acetic acid
Publikations- och innehållstyp
- art (ämneskategori)
- ref (ämneskategori)
Hitta via bibliotek
Till lärosätets databas
- Av författaren/redakt...
-
Tissot, H.
-
Halldin Stenlid, ...
-
Wang, C.
-
Panahi, M.
-
Kaya, S.
-
Brinck, T.
-
visa fler...
-
Sassa, Yasmine, ...
-
Johansson, Fredr ...
-
Weissenrieder, J ...
-
visa färre...
- Om ämnet
-
- NATURVETENSKAP
-
NATURVETENSKAP
-
och Kemi
-
och Oorganisk kemi
-
- NATURVETENSKAP
-
NATURVETENSKAP
-
och Kemi
-
och Annan kemi
-
- NATURVETENSKAP
-
NATURVETENSKAP
-
och Kemi
-
och Organisk kemi
- Artiklar i publikationen
-
Journal of Catal ...
- Av lärosätet
-
Chalmers tekniska högskola