Abstract
Activation of carbon dioxide is the most important step in its conversion into valuable chemicals. Surfaces of stable oxide with a low work function may be promising for this purpose. Here we report that the surfaces of the inorganic electride [Ca24Al28O64]4+(e -)4 activate and split carbon dioxide at room temperature. This behaviour is attributed to a high concentration of localized electrons in the near-surface region and a corrugation of the surface that can trap oxygen atoms and strained carbon monoxide and carbon dioxide molecules. The [Ca 24Al28O64]4+(e-) 4 surface exposed to carbon dioxide is studied using temperature-programmed desorption, and spectroscopic methods. The results of these measurements, corroborated with ab initio simulations, show that both carbon monoxide and carbon dioxide adsorb on the [Ca24Al 28O64]4+(e-)4 surface at RT and above and adopt unusual configurations that result in desorption of molecular carbon monoxide and atomic oxygen upon heating.
| Original language | English |
|---|---|
| Article number | 2378 |
| Journal | Nature Communications |
| Volume | 4 |
| DOIs | |
| Publication status | Published - 1 Dec 2013 |
| Externally published | Yes |
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ASJC Scopus subject areas
- Biochemistry, Genetics and Molecular Biology(all)
- Chemistry(all)
- Physics and Astronomy(all)
Cite this
Activation and splitting of carbon dioxide on the surface of an inorganic electride material. / Toda, Yoshitake; Hirayama, Hiroyuki; Kuganathan, Navaratnarajah; Torrisi, Antonio; Sushko, Peter V.; Hosono, Hideo.
In: Nature Communications, Vol. 4, 2378, 01.12.2013.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Activation and splitting of carbon dioxide on the surface of an inorganic electride material
AU - Toda, Yoshitake
AU - Hirayama, Hiroyuki
AU - Kuganathan, Navaratnarajah
AU - Torrisi, Antonio
AU - Sushko, Peter V.
AU - Hosono, Hideo
PY - 2013/12/1
Y1 - 2013/12/1
N2 - Activation of carbon dioxide is the most important step in its conversion into valuable chemicals. Surfaces of stable oxide with a low work function may be promising for this purpose. Here we report that the surfaces of the inorganic electride [Ca24Al28O64]4+(e -)4 activate and split carbon dioxide at room temperature. This behaviour is attributed to a high concentration of localized electrons in the near-surface region and a corrugation of the surface that can trap oxygen atoms and strained carbon monoxide and carbon dioxide molecules. The [Ca 24Al28O64]4+(e-) 4 surface exposed to carbon dioxide is studied using temperature-programmed desorption, and spectroscopic methods. The results of these measurements, corroborated with ab initio simulations, show that both carbon monoxide and carbon dioxide adsorb on the [Ca24Al 28O64]4+(e-)4 surface at RT and above and adopt unusual configurations that result in desorption of molecular carbon monoxide and atomic oxygen upon heating.
AB - Activation of carbon dioxide is the most important step in its conversion into valuable chemicals. Surfaces of stable oxide with a low work function may be promising for this purpose. Here we report that the surfaces of the inorganic electride [Ca24Al28O64]4+(e -)4 activate and split carbon dioxide at room temperature. This behaviour is attributed to a high concentration of localized electrons in the near-surface region and a corrugation of the surface that can trap oxygen atoms and strained carbon monoxide and carbon dioxide molecules. The [Ca 24Al28O64]4+(e-) 4 surface exposed to carbon dioxide is studied using temperature-programmed desorption, and spectroscopic methods. The results of these measurements, corroborated with ab initio simulations, show that both carbon monoxide and carbon dioxide adsorb on the [Ca24Al 28O64]4+(e-)4 surface at RT and above and adopt unusual configurations that result in desorption of molecular carbon monoxide and atomic oxygen upon heating.
UR - http://www.scopus.com/inward/record.url?scp=84893365376&partnerID=8YFLogxK
U2 - 10.1038/ncomms3378
DO - 10.1038/ncomms3378
M3 - Article
VL - 4
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
M1 - 2378
ER -