Catàlisi Predictiva per la Generació d’H2 a partir d'Etilenglicol i Amines

Abstract

The objective of this project is to study, from a computational chemistry perspective and

considering the principles of green chemistry, the reaction for the synthesis of

oxalamides. These molecules are used in medicine as anticoagulants and have also been

observed to have good antiviral activity. For this reason, it is important to determine a

way to soften the conditions for their formation and generate less waste. To carry out

this study, we will base our approach on an article about the synthesis of oxalamides by

acceptorless dehydrogenative coupling of ethylene glycol and amines and the reverse

hydrogenation catalyzed by ruthenium.

In the experimental work by Milstein et al., they have successfully synthesized

oxalamides in a sustainable way, generating only H₂ as a byproduct.

We will study this catalyst using computational methods, specifically Density Functional

Theory (DFT), with the use of Gaussian 16 and ChemCraft software. To carry out this

project, we will modify different functional groups of the ruthenium catalyst to observe

if it is possible to decrease its activation energy in the rate-determining step of the

reaction mechanism. To achieve this, we will study the minimum and the transition state

determinants of each modification made to the catalyst, first in the gas phase by

optimizing its geometry, and then with a single-point calculation considering the effect

of the solvent. We will use the BP86 functional and the Def2SVP basis set for the gas

phase calculations, and the B3LYP functional with the Def2TZVP basis set for the

calculations that consider the solvent