ab-Initio Study of Hydrogen Bond Networks in 1,2,3-Triazole Phases

Abstract

The research in storage and conversion of energy is an everlasting process. The use of fuel cells is very tempting but up to now there are still several conceptual challenges to overcome. Especially, the requirement of liquid water causes difficulties due to the temperature limit. Therefore, imidazoles and triazoles are increasingly investigated in a manifold of experimental and theoretical publications as they are both very promising in overcoming this problem. Recently, triazoles were found to be superior to imidazoles in proton conduction. An ab-initio molecular dynamics simulation of pure triazole phases for investigating the behavior of both tautomer species of the triazole molecule has never been done. In this work, we investigate the structural and dynamical properties of two different solid phases and the liquid phase at two different temperatures. We are able to show how the distinct tautomers contribute to the mechanism of proton conduction, to compute dynamical properties of the four systems and to suggest a mechanism of reorientation in solid phase.

Intermolecular interactions in clusters of ethylammonium nitrate and 1-amino-1,2,3-triazole

“…121 The resulting H-bond H42⋯N18 distance is 2.09Å, in good agreement with the dispersion driven intermolecular H-bonds observed in a previous study. 121…”

“…The distance between the two centers of mass of the two 1-AT molecules is 4.34 Å, which falls in the distance range reported by Peschel and coworkers. 121 The resulting H-bond H42Á Á ÁN18 distance is 2.09Å, in good agreement with the dispersion driven intermolecular H-bonds observed in a previous study. 121 The EFP-optimized structure of (EAN) 1 :(1-AT) 4 (Fig.…”

“…121 The resulting H-bond H42Á Á ÁN18 distance is 2.09Å, in good agreement with the dispersion driven intermolecular H-bonds observed in a previous study. 121 The EFP-optimized structure of (EAN) 1 :(1-AT) 4 (Fig. 7d) shows that three 1-AT molecules form H-bonds with the EAN monomer, while the fourth 1-AT molecule does not have an H-bond interaction with the other molecules in the cluster.…”

“…The H-bond interaction between two 1-AT molecules can be driven by dispersion interactions. According to the H-bond analysis done by Peschel and coworkers 121 using ab initio molecular dynamics with the GTH-BLYP functional, intermolecular H-bonds between two 1,2,3-triazole molecules with p-p interactions were observed under specific conditions: two triazole molecules were arranged in a (parallel) sandwich configuration to maximize the p-p interactions with a distance between the two centers of mass of 3.7 to 5 Å. 121 The intermolecular H-bond was formed between a hydrogen atom (bonded to a nitrogen atom on the hetero aromatic ring) on one 1,2,3-triazole and a nitrogen atom in the aromatic ring on the other 1,2,3-triazole.…”