Abstract
We present adsorption processes of dinitrogen on size-selected silver cluster cations, Agn+ (n = 1–10), studied by kinetics measurement using an ion trap. The cluster ions showed sequential adsorption of N2 molecules when the ion trap was cooled down to 105 K, excluding n = 8 and 9 that were exceptionally inactive at this temperature. Termolecular rate coefficients of each adsorption step are determined by analyzing time-dependent changes in the reactant and product ion signals. The first-step rate coefficients were found to increase exponentially from n = 1 to 7 due to increased internal degrees of freedom at larger sizes, which are favorable for accommodating the adsorption energy in a free cluster. In contrast, the adsorption rate turned to decrease for n > 7 due to weaker binding of dinitrogen as revealed by density-functional-theory (DFT) calculation. Adsorption sites on Agn+ are further discussed on the basis of the maximum number of adsorbing N2 molecules observed in the experiment.
Acknowledgements
T.I. appreciates the Grant-in-Aid for JSPS Fellows (Funder Id: http://dx.doi.org/10.13039/501100001691, JP13J06463) from the Japan Society for Promotion of Science (JSPS). The present study was supported by the Grant-in-Aid for Scientific Research (A) (Funder Id: http://dx.doi.org/10.13039/501100001691, JP23245006) from JSPS. The DFT calculations were performed mainly by the computing system at the Research Institute for Information Technology, Kyushu University.
References
1. M. Haruta, T. Kobayashi, H. Sano, N. Yamada, Chem. Lett. 16 (1987) 405.10.1246/cl.1987.405Search in Google Scholar
2. P. J. Roach, W.H. Woodward, A. W. Castleman Jr., A. C. Reber, S. N. Khanna, Science 323 (2009) 492.10.1126/science.1165884Search in Google Scholar PubMed
3. W. H. Woodward, A. C. Reber, J. C. Smith, S. N. Khanna, A. W. Castleman Jr., J. Phys. Chem. C 117 (2013) 7445.10.1021/jp303668bSearch in Google Scholar
4. M. Arakawa, R. Yamane, A. Terasaki, J. Phys. Chem. A 120 (2016) 139.10.1021/acs.jpca.5b08900Search in Google Scholar PubMed
5. M. Arakawa, T. Omoda, A. Terasaki, J. Phys. Chem. C 121 (2017) 10790.10.1021/acs.jpcc.6b11689Search in Google Scholar
6. J. Ma, X. Cao, X. Xing, X. Wang, J. H. Parks, Phys. Chem. Chem. Phys. 18 (2016) 743.10.1039/C5CP06116DSearch in Google Scholar PubMed
7. V. Bonačić-Koutecký, L. Češpiva, P. Fantucci, J. Koutecký, J. Chem. Phys. 98 (1993) 7981.10.1063/1.464552Search in Google Scholar
8. M. L. McKee, A. Samokhvalov, J. Phys. Chem. A 121 (2017) 5018.10.1021/acs.jpca.7b03905Search in Google Scholar PubMed
9. P. Weis, T. Bierweiler, S. Gilb, M. M. Kappes, Chem. Phys. Lett. 355 (2002) 355.10.1016/S0009-2614(02)00277-4Search in Google Scholar
10. T. van der Tol, D. Jia, Y. Li, V. Chernyy, J. M. Bakker, et al., Phys. Chem. Chem. Phys. 19 (2017) 19360.10.1039/C7CP03335DSearch in Google Scholar PubMed
11. M. J. Manard, P. R. Kemper, M. T. Bowers, J. Am. Chem. Soc. 127 (2005) 9994.10.1021/ja052251jSearch in Google Scholar PubMed
12. M. Schmidt, A. Masson, H.-P. Cheng, C. Bréchignac, Chem. Phys. Chem. 16 (2015) 855.10.1002/cphc.201402726Search in Google Scholar PubMed
13. Y. N. Wu, M. Schmidt, J. Leygnier, H. P. Cheng, A. Masson, et al., J. Chem. Phys. 136 (2012) 024314.10.1063/1.3673616Search in Google Scholar PubMed
14. M. Schmidt, A. Masson, C. Bréchignac, J. Chem. Phys. 122 (2005) 134712.10.1063/1.1871892Search in Google Scholar PubMed
15. M. Schmidt, A. Masson, C. Bréchignac, Phys. Rev. Lett. 91 (2003) 243401.10.1103/PhysRevLett.91.243401Search in Google Scholar PubMed
16. D. Schooss, S. Gilb, J. Kaller, M. M. Kappes, F. Furche, et al., J. Chem. Phys. 113 (2000) 5361; ibid. 113 (2000) 10413.10.1063/1.1290028Search in Google Scholar
17. G. Naresh Patwari, T. Ito, K. Egashira, A. Terasaki, Chem. Asian J. 6 (2011) 1834.10.1002/asia.201000901Search in Google Scholar PubMed
18. F. Mafuné, Y. Tawaraya, S. Kudoh, J. Phys. Chem. A 120 (2016) 4089.10.1021/acs.jpca.6b03479Search in Google Scholar PubMed
19. M. P. Klein, A. A. Ehrhard, J. Mohrbach, S. Dillinger, G. Niedner-Schatteburg, Top. Catal. 61 (2018) 106.10.1007/s11244-017-0865-2Search in Google Scholar
20. S. Dillinger, J. Mohrbach, J. Hewer, M. Gaffga, G. Niedner-Schatteburg, Phys. Chem. Chem. Phys. 17 (2015) 10358.10.1039/C5CP00047ESearch in Google Scholar PubMed
21. J. Mohrbach, S. Dillinger, G. Niedner-Schatteburg, J. Phys. Chem. C 121 (2017) 10907.10.1021/acs.jpcc.6b12167Search in Google Scholar
22. J. Mohrbach, S. Dillinger, G. Niedner-Schatteburg, J. Chem. Phys. 147 (2017) 184304.10.1063/1.4997403Search in Google Scholar PubMed
23. S. Dillinger, J. Mohrbach, G. Niedner-Schatteburg, J. Chem. Phys. 147 (2017) 184305.10.1063/1.4997407Search in Google Scholar PubMed
24. A. Terasaki, T. Majima, T. Kondow, J. Chem. Phys. 127 (2007) 231101.10.1063/1.2822022Search in Google Scholar PubMed
25. T. Ito, K. Egashira, K. Tsukiyama, A. Terasaki, Chem. Phys. Lett. 538 (2012) 19.10.1016/j.cplett.2012.04.040Search in Google Scholar
26. M. Arakawa, K. Ando, S. Fujimoto, S. Mishra, G. Naresh Patwari, et al., Phys. Chem. Chem. Phys. 20 (2018) 13974.10.1039/C8CP00424BSearch in Google Scholar PubMed
27. A. D. Becke, J. Chem. Phys. 98 (1993) 5648.10.1063/1.464913Search in Google Scholar
28. C. Lee, W. Yang, R. G. Parr, Phys. Rev. B 37 (1988) 785.10.1103/PhysRevB.37.785Search in Google Scholar
29. M. Couty, M. B. Hall, J. Comp. Chem. 17 (1996) 1359.10.1002/(SICI)1096-987X(199608)17:11<1359::AID-JCC9>3.0.CO;2-LSearch in Google Scholar
30. T. H. Dunning Jr., J. Chem. Phys. 90 (1989) 1007.10.1063/1.456153Search in Google Scholar
31. R. A. Kendall, T. H. Dunning Jr., R. J. Harrison, J. Chem. Phys. 96 (1992) 6796.10.1063/1.462569Search in Google Scholar
32. M. J. Frisch, G. W. Trucks, H. B. Schlegel, G. E. Scuseria, M. A. Robb, et al., Gaussian 16, Revision A.03, Gaussian, Inc., Wallingford, CT (2016).Search in Google Scholar
33. E. Schumacher, DETMECH – chemical reaction kinetics software. Chemistry Department, University of Bern, Switzerland (2003).Search in Google Scholar
34. T. M. Bernhardt, J. Hagen, S. M. Lang, D. M. Popolan, L. D. Socaciu-Siebert, et al., J. Phys. Chem. A 113 (2009) 2724.10.1021/jp810055qSearch in Google Scholar PubMed
35. J. L. F. Da Silva, C. Stampfl, M. Scheffler, Phys. Rev. Lett. 90 (2003) 066104.10.1103/PhysRevLett.90.066104Search in Google Scholar PubMed
Supplementary Material
The online version of this article offers supplementary material (DOI: https://doi.org/10.1515/zpch-2019-1373).
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