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要旨:
The course of the Diels-Alder reactions of cyclopentadiene and maleic
anhydride were studied. Two reaction paths were modelled: endo-and
exo-selective paths. All structures within the transient region were
characterized and analyzed by means of geometrical descriptors,
physicochemical parameters and information-theoretical measures in order
to observe the linkage between chemical behavior and the carriage of
information. We have shown that the information-theoretical
characterization of the chemical course of the reaction is in complete
agreement with its phenomenological behavior in passing from reactants
to products. In addition, we were able to detect the main differences
between the two reaction mechanisms. This type of informational analysis
serves to provide tools to help understand the chemical reactivity of
the two simplest Diels-Alder reactions, which permits the establishment
of a connection between the quantum changes that molecular systems exert
along reaction coordinates and standard physicochemical phenomenology.
In the present study, we have shown that every reaction stage has a
family of subsequent structures that are characterized not solely by
their phenomenological behavior but also by informational properties of
their electronic density distribution (localizability, order,
uniformity). Moreover, we were able to describe the main differences
between endo-adduct and exo-adduct pathways. With the advent of new
experimental techniques, it is in principle possible to observe the
structural changes in the transient regions of chemical reactions.
Indeed, through this work we have provided the theoretical concepts
needed to unveil the concurrent processes associated with chemical
reactions.
