Actas de congresos
On The Dynamics Of Graphdiyne Hydrogenation
Registro en:
9781605115269
Materials Research Society Symposium Proceedings. Materials Research Society, v. 1549, n. , p. 59 - 64, 2013.
2729172
10.1557/opl.2013.608
2-s2.0-84898474392
Autor
Autreto P.A.
De Sousa J.M.
Galvao D.S.
Institución
Resumen
Graphene is a two-dimensional (2D) hexagonal array of carbon atoms in sp2-hybridized states. Graphene presents unique and exceptional electronic, thermal and mechanical properties. However, in its pristine state graphene is a gapless semiconductor, which poses some limitations to its use in some transistor electronics. Because of this there is a renewed interest in other possible two-dimensional carbon-based structures similar to graphene. Examples of mis are graphynes and graphdiynes, which are two-dimensional structures, composed of carbon atoms in sp2 and sp-hybridized states. Graphdiynes (benzenoid rings connecting two acetylenic groups) were recently synthesized and they can be intrinsically nonzero gap systems. These systems can be easily hydrogenated and the amount of hydrogenation can be used to tune the band gap value. In this work we have investigated, through fully atomistic molecular dynamics simulations with reactive force field (ReaxFF), the structural and dynamics aspects of the hydrogenation mechanisms of graphdiyne membranes. Our results showed that depending on whether the atoms are in the benzenoid rings or as part of the acetylenic groups, the rates of hydrogenation are quite distinct and change in time in a very complex pattern. Initially, the most probable sites to be hydrogenated are the carbon atoms forming the triple bonds, as expected. But as the amount of hydrogenation increases in time this changes and then the carbon atoms forming single bonds become the preferential sites. The formation of correlated domains observed in hydrogenated graphene is no longer observed in the case of graphdiynes. We have also carried out ab initio DFT calculations for model structures in order to test the reliability of ReaxFF calculations. © 2013 Materials Research Society. 1549
59 64 Novoselov, K.S., (2004) Science, 306, p. 666 Cheng, S.H., (2010) Phys. Rev. B, 81, p. 205435 Malko, D., Neiss, C., Vines, F., Gorling, A., (2012) Phys. Rev. Lett., 108, p. 086804 Baughman, R., Eckhardt, H., Kertesz, M., (1987) J. Chem. Phys., 87, p. 6687 Peng, Q., Ji, W., De, S., (2012) Phys. Chem. Chem. Phys., 14, p. 13385 Coluci, V.R., Braga, S.F., Legoas, S.B., Galvao, D.S., Baughman, R.H., (2003) Phys. Rev. B, 68, p. 035430 Coluci, V.R., Braga, S.F., Legoas, S.B., Galvao, D.S., Baughman, R.H., (2004) Nanotechnology, 15, p. 8142 Li, G., (2010) Chem. Commun., 46, p. 3256 Luo, G., (2011) Phys. Rev. B, 84, p. 075439 Psofogiannakis, G.M., Froudakis, G.E., (2012) J. Phys. Chem. C, 116, p. 19211 Flores, M.Z.S., Autreto, P.A.S., Legoas, S.B., Galvao, D.S., (2009) Nanotechnology, 20, p. 465704 Cranford, S.W., Buelher, M.J., (2012) Nanoscale, 4, p. 4587 Van Duin, A.C.T., Dasgupta, S., Lorant, F., Goddard III, W.A., (2001) J. Phys. Chem. A, 105, p. 9396 Van Duin, A.C.T., Damste, J.S.S., (2003) Org. Geochem., 34, p. 515 Chenoweth, K., Van Duin, A.C.T., Goddard III, W.A., (2008) J. Phys. Chem. A, 112, p. 1040 Plimpton, S., (1995) J. Comp. Phys., 117, p. 1. , http://lammps.sandia.gov/ Delly, B., (1990) J. Chem. Phys., 92, p. 508 Perdew, J., Burke, K., Ernzerhof, M., (1996) Phys. Rev. Lett., 77, p. 3865 Paupitz, R., (2013) Nanotechnology, 24, p. 035706