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  Size-Specific, Dissociative Activation of Carbon Dioxide by Cobalt Cluster Anions

Yanagimachi, A., Koyasu, K., Valdivielso, D. Y., Gewinner, S., Schöllkopf, W., Fielicke, A., et al. (2016). Size-Specific, Dissociative Activation of Carbon Dioxide by Cobalt Cluster Anions. The Journal of Physical Chemistry C, 120(26), 14209-14215. doi:10.1021/acs.jpcc.6b04360.

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Yanagimachi, Akimaro 1, Author
Koyasu, Kiichirou 1, 2, Author
Valdivielso, David Yubero 3, Author
Gewinner, Sandy4, Author              
Schöllkopf, Wieland4, Author              
Fielicke, André 3, Author
Tsukuda, Tatsuya 1, 2, Author
Affiliations:
1Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan, ou_persistent22              
2Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, Katsura, Kyoto 615-8520, Japan, ou_persistent22              
3Institut für Optik und Atomare Physik, Technische Universität Berlin, Hardenbergstr. 36, D-10623 Berlin, Germany, ou_persistent22              
4Molecular Physics, Fritz Haber Institute, Max Planck Society, ou_634545              

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 Abstract: The reaction of cobalt cluster anions Con (3 ≤ n ≤ 17) with CO2 was studied experimentally and theoretically to explore the size-specific activation mode of CO2 by Con. Mass spectrometric measurements revealed that the reactivity depends strongly on cluster size: the reactivity emerges abruptly at n = 7, peaks at n = 8–10, and then gradually decreases with increasing n. Infrared multiple photon dissociation spectra of ConCO2 exhibit a single peak at ∼1870 cm–1, similarly to the previously reported spectra of ConCO. Density functional theory calculations for Co7CO2 as an example revealed that the dissociative adsorption of CO2 into CO and O is energetically more favorable than nondissociative adsorption. The infrared spectra calculated for dissociated isomers Co7(CO)O reproduced the experimental results, whereas those for nondissociated isomers Co7CO2 did not. The photoelectron spectra of ConCO2 were shifted dramatically toward higher energies relative to those of Con, suggesting electron transfer from Con to the CO and O ligands. These results indicate that the CO2 molecule adsorbs dissociatively on Con, in sharp contrast to its nondissociative adsorption onto the Co monomer anion.

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 Dates: 2016-06-132016-04-292016-06-132016-07-07
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jpcc.6b04360
 Degree: -

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Title: The Journal of Physical Chemistry C
  Abbreviation : J. Phys. Chem. C
Source Genre: Journal
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Publ. Info: Washington DC : American Chemical Society
Pages: 7 Volume / Issue: 120 (26) Sequence Number: - Start / End Page: 14209 - 14215 Identifier: ISSN: 1932-7447
CoNE: https://pure.mpg.de/cone/journals/resource/954926947766