Rotational Characterization of an n → π* Interaction in a Pyridine–Formaldehyde Adduct

The rotational spectrum of the pyridine–formaldehyde adduct generated in a supersonic expansion has been analyzed using Fourier transform microwave spectroscopy. The spectrum shows the quadrupole coupling hyperfine structure due to the presence of 14N. The spectra of the parent, 13C and 15N isotopol...

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Detalles Bibliográficos
Autores: Blanco Rodríguez, Susana, López Alonso, Juan Carlos
Tipo de recurso: artículo
Estado:Versión borrador
Fecha de publicación:2018
País:España
Institución:Universidad de Valladolid
Repositorio:UVaDOC. Repositorio Documental de la Universidad de Valladolid
OAI Identifier:oai:uvadoc.uva.es:10324/46299
Acceso en línea:https://doi.org/10.1021/acs.jpclett.8b01719
http://uvadoc.uva.es/handle/10324/46299
Access Level:acceso abierto
Palabra clave:Espectroscopía de rotación
Quimica
rotational spectroscopy
structure
non covalent interaction
n - pi interaction
pyridine - formaldehyde
molecular complexes
23 Química
2301.13 Espectroscopia de Microondas
2307 Química Física
Descripción
Sumario:The rotational spectrum of the pyridine–formaldehyde adduct generated in a supersonic expansion has been analyzed using Fourier transform microwave spectroscopy. The spectrum shows the quadrupole coupling hyperfine structure due to the presence of 14N. The spectra of the parent, 13C and 15N isotopologues have been observed to investigate its structure. The complex shows a Cs symmetry with the plane of pyridine bisecting the <HCH angle of formaldehyde and the N atom located along the Bürgi-Dunitz trajectory of nucleophile addition to a carbonyl group (r(N-C)=2.855(4) Å, <NC=O=102.8(6)º). From this structure and with the help of ab initio computations and natural bond orbital analysis it is shown unambiguously that pyridine links to formaldehyde, the smallest molecule bearing a carbonyl group, through an n->pi* interaction together with a weak C-H...O bond.