dc.contributor.author | Flórez E | |
dc.contributor.author | Acelas N | |
dc.contributor.author | Gómez S | |
dc.contributor.author | Hadad C | |
dc.contributor.author | Restrepo A. | |
dc.date.accessioned | 2022-09-14T14:34:17Z | |
dc.date.available | 2022-09-14T14:34:17Z | |
dc.date.created | 2022 | |
dc.identifier.issn | 14394235 | |
dc.identifier.uri | http://hdl.handle.net/11407/7607 | |
dc.description | A detailed analysis under a comprehensive set of theoretical and computational tools of the thermodynamical factors and of the intermolecular interactions behind the stabilization of a well known set of (water)20 cavities and of the methane clathrate is offered in this work. Beyond the available reports of experimental characterization at extreme conditions of most of the systems studied here, all clusters should be amenable to experimental detection at 1 atm and moderate temperatures since 280 K marks the boundary at which, ignoring reaction paths, formation of all clusters is no longer spontaneous from the 20H2O→(H2O)20 and CH4+20H2O→CH4@512 processes. As a function of temperature, a complex interplay leading to the free energy of formation occurs between the destabilizing entropic contributions, mostly due to cluster vibrations, and the stabilizing enthalpic contributions, due to intermolecular interactions and the PV term, is best illustrated by the highly symmetric 512 cage consistently showing signs of stronger intermolecular bonding despite having smaller binding energy than the other clusters. A fluxional wall of attractive non-covalent interactions, arising because of the cumulative effect of a large number of tiny individual charge transfers to the interstitial region, plays a pivotal role stabilizing the CH4@512 clathrate. © 2021 Wiley-VCH GmbH | eng |
dc.language.iso | eng | |
dc.publisher | John Wiley and Sons Inc | |
dc.relation.isversionof | https://www.scopus.com/inward/record.uri?eid=2-s2.0-85122803420&doi=10.1002%2fcphc.202100716&partnerID=40&md5=a09c75848f51f94748e8df8c93ed3dce | |
dc.source | ChemPhysChem | |
dc.title | To Be or Not To Be? that is the Entropic, Enthalpic, and Molecular Interaction Dilemma in the Formation of (Water)20 Clusters and Methane Clathrate | |
dc.type | Article | |
dc.rights.accessrights | info:eu-repo/semantics/restrictedAccess | |
dc.publisher.program | Ciencias Básicas | |
dc.type.spa | Artículo | |
dc.identifier.doi | 10.1002/cphc.202100716 | |
dc.subject.keyword | Charge transfer | eng |
dc.subject.keyword | Free energy | eng |
dc.subject.keyword | Hydration | eng |
dc.subject.keyword | Methane | eng |
dc.subject.keyword | CH 4 | eng |
dc.subject.keyword | Computational tools | eng |
dc.subject.keyword | Experimental characterization | eng |
dc.subject.keyword | Extreme conditions | eng |
dc.subject.keyword | Intermolecular interactions | eng |
dc.subject.keyword | Methane clathrates | eng |
dc.subject.keyword | Moderate temperature | eng |
dc.subject.keyword | Path formation | eng |
dc.subject.keyword | Reaction paths | eng |
dc.subject.keyword | Thermodynamical | eng |
dc.subject.keyword | Binding energy | eng |
dc.relation.citationvolume | 23 | |
dc.relation.citationissue | 2 | |
dc.publisher.faculty | Facultad de Ciencias Básicas | |
dc.affiliation | Flórez, E., Grupo de Materiales con Impacto (Mat&mpac), Facultad de Ciencias Básicas, Universidad de Medellín, Medellín, Colombia | |
dc.affiliation | Acelas, N., Grupo de Materiales con Impacto (Mat&mpac), Facultad de Ciencias Básicas, Universidad de Medellín, Medellín, Colombia | |
dc.affiliation | Gómez, S., Scuola Normale Superiore, Classe di Scienze, Piazza dei Cavalieri 7, Pisa, 56126, Italy | |
dc.affiliation | Hadad, C., Instituto de Química, Universidad de Antioquia UdeA, Calle 70 No. 52–21, Medellín, Colombia | |
dc.affiliation | Restrepo, A., Instituto de Química, Universidad de Antioquia UdeA, Calle 70 No. 52–21, Medellín, Colombia | |
dc.relation.references | Samanta, D., Klajn, R., (2017) Science, 355, p. 912 | |
dc.relation.references | Takeya, S., Uchida, T., Kamata, Y., Nagao, J., Kida, M., Minami, H., Sakagami, H., Soloviev, V., (2005) Angew. Chem. Int. Ed., 44, pp. 6928-6931 | |
dc.relation.references | (2005) Angew. Chem., 117, pp. 7088-7091 | |
dc.relation.references | Nguyen, N.N., Berger, R., Wagner, M., Thiel, J., Butt, H.-J., Graf, R., (2021) J. Phys. Chem. C, 125, pp. 15751-15757 | |
dc.relation.references | Huang, Y., Zhu, C., Wang, L., Cao, X., Su, Y., Jiang, X., Meng, S., Zeng, X.C., (2016) Sci. Adv., 2 | |
dc.relation.references | Shin, K., Moudrakovski, I.L., Ratcliffe, C.I., Ripmeester, J.A., (2017) Angew. Chem. Int. Ed., 56, pp. 6171-6175 | |
dc.relation.references | (2017) Angew. Chem., 129, pp. 6267-6271 | |
dc.relation.references | Alavi, S., Ripmeester, J.A., (2007) Angew. Chem. Int. Ed., 46, pp. 6102-6105 | |
dc.relation.references | (2007) Angew. Chem., 119, pp. 6214-6217 | |
dc.relation.references | Walsh, M.R., Koh, C.A., Sloan, E.D., Sum, A.K., Wu, D.T., (2009) Science, 326, pp. 1095-1098 | |
dc.relation.references | Ludwig, R., Appelhagen, A., (2005) Angew. Chem. Int. Ed., 44, pp. 811-815 | |
dc.relation.references | (2005) Angew. Chem., 117, pp. 821-826 | |
dc.relation.references | Shin, K., Udachin, K.A., Moudrakovski, I.L., Leek, D.M., Alavi, S., Ratcliffe, C.I., Ripmeester, J.A., (2013) Proc. Natl. Acad. Sci. USA, 110, pp. 8437-8442 | |
dc.relation.references | Yoo, C.-S., (2017) MRS Bull., 42, pp. 724-728 | |
dc.relation.references | Luspay-Kuti, A., Mousis, O., Hässig, M., Fuselier, S.A., Lunine, J.I., Marty, B., Mandt, K.E., Rubin, M., (2016) Sci. Adv., 2 | |
dc.relation.references | Chattaraj, P.K., Bandaru, S., Mondal, S., (2011) J. Phys. Chem. A, 115, pp. 187-193 | |
dc.relation.references | Buch, V., Devlin, J.P., Monreal, I.A., Jagoda-Cwiklik, B., Uras-Aytemiz, N., Cwiklik, L., (2009) Phys. Chem. Chem. Phys., 11, pp. 10245-10265 | |
dc.relation.references | Falenty, A., Hansen, T.C., Kuhs, W.F., (2014) Nature, 516, pp. 231-233 | |
dc.relation.references | Ghosh, J., Methikkalam, R.R.J., Bhuin, R.G., Ragupathy, G., Choudhary, N., Kumar, R., Pradeep, T., (2019) Proc. Natl. Acad. Sci. USA, 116, pp. 1526-1531 | |
dc.relation.references | Ghosh, J., Bhuin, R.G., Vishwakarma, G., Pradeep, T., (2020) J. Chem. Phys., 11, pp. 26-32 | |
dc.relation.references | Wei, S., Shi, Z., Castleman, A.W., (1991) J. Chem. Phys., 94, pp. 3268-3270 | |
dc.relation.references | Bader, R., (1990) Atoms in Molecules: A Quantum Theory, , Oxford Univ. press Oxford | |
dc.relation.references | Popelier, P.L., (2000) Atoms in Molecules: An Introduction, , Prentice Hall, London | |
dc.relation.references | Grabowski, S.J., (2011) Chem. Rev., 111, pp. 2597-2625 | |
dc.relation.references | Reed, A.E., Curtiss, L.A., Weinhold, F., (1988) Chem. Rev., 88, pp. 899-926 | |
dc.relation.references | Weinhold, F., Landis, C., Glendening, E., (2016) Int. Rev. Phys. Chem., 35, pp. 399-440 | |
dc.relation.references | Weinhold, F., Landis, C.R., (2012) Discovering Chemistry with Natural Bond Orbitals, , Wiley-VCH, Hoboken NJ, 319 pp | |
dc.relation.references | Johnson, E.R., Keinan, S., Mori-Sánchez, P., Contreras-García, J., Cohen, A.J., Yang, W., (2010) J. Am. Chem. Soc., 132, pp. 6498-6506 | |
dc.relation.references | DiLabio, G.A., Otero-de-la Roza, A., (2016) Reviews in Computational Chemistry, pp. 1-97. , John Wiley & Sons, Ltd., Chapter 1, pp | |
dc.relation.references | Wang, K., Li, W., Li, S., (2014) J. Chem. Theory Comput., 10, pp. 1546-1553 | |
dc.relation.references | Gaussian Inc (2009) Wallingford CT | |
dc.relation.references | (2013) NBO 6.0, , Theoretical Chemistry Institute, University of Wisconsin, Madison | |
dc.relation.references | (2019) AIMALL (Version 19.10.12), , TK Gristmill Software, Overland Park KS, USA, aim.tkgristmill.com | |
dc.relation.references | Contreras-García, J., Johnson, E.R., Keinan, S., Chaudret, R., Piquemal, J.-P., Beratan, D.N., Yang, W., (2011) J. Chem. Theory Comput., 7, pp. 625-632 | |
dc.relation.references | Pal, J., Patla, A., Subramanian, R., (2021) Chemosphere, 272 | |
dc.relation.references | Stachl, C.N., Williams, E.R., (2020) J. Chem. Phys., 11, pp. 6127-6132 | |
dc.relation.references | Johnson, R., (2002) | |
dc.relation.references | Rojas-Valencia, N., Gómez, S., Guerra, D., Restrepo, A., (2020) Phys. Chem. Chem. Phys., 22, pp. 13049-13061 | |
dc.relation.references | Gómez, S.A., Rojas-Valencia, N., Gómez, S., Egidi, F., Cappelli, C., Restrepo, A., (2021) ChemBioChem, 22, pp. 724-732 | |
dc.relation.references | Gomez, S.A., Rojas-Valencia, N., Gomez, S., Cappelli, C., Restrepo, A., Chembiochem, , https://doi.org/10.1002/cbic.202100393 | |
dc.relation.references | Rojas-Valencia, N., Gómez, S., Montillo, S., Manrique-Moreno, M., Cappelli, C., Hadad, C., Restrepo, A., (2020) J. Phys. Chem. B, 124, pp. 79-90 | |
dc.relation.references | Rojas-Valencia, N., Gómez, S., Núñez-Zarur, F., Cappelli, C., Hadad, C., Restrepo, A., (2021) J. Phys. Chem. B, 125, pp. 10383-10391 | |
dc.relation.references | Keutsch, F.N., Saykally, R.J., (2001) Proc. Natl. Acad. Sci. USA, 98, pp. 10533-10540 | |
dc.relation.references | Flórez, E., Acelas, N., Ramírez, F., Hadad, C., Restrepo, A., (2018) Phys. Chem. Chem. Phys., 20, pp. 8909-8916 | |
dc.relation.references | David, J., Gomez, S., Guerra, D., Guerra, D., Restrepo, A., (2021) ChemPhysChem | |
dc.relation.references | Cuautli, C., Hernández-Lamoneda, R., (2019) J. Phys. Chem. C, 123, pp. 24793-24806 | |
dc.relation.references | Gómez, S., Rojas-Valencia, N., Gómez, S.A., Cappelli, C., Merino, G., Restrepo, A., (2021) Chem. Sci., 12, pp. 9233-9245 | |
dc.relation.references | Gómez, S., Nafziger, J., Restrepo, A., Wasserman, A., (2017) J. Chem. Phys., 146 | |
dc.relation.references | Hincapié, G., Acelas, N., Castaño, M., David, J., Restrepo, A., (2010) J. Phys. Chem. A, 114, pp. 7809-7814 | |
dc.type.coar | http://purl.org/coar/resource_type/c_6501 | |
dc.type.version | info:eu-repo/semantics/publishedVersion | |
dc.type.driver | info:eu-repo/semantics/article | |
dc.identifier.reponame | reponame:Repositorio Institucional Universidad de Medellín | |
dc.identifier.repourl | repourl:https://repository.udem.edu.co/ | |
dc.identifier.instname | instname:Universidad de Medellín | |