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Isomers are different chemical species that have the same chemical formula. Structural isomerism of coordination compounds can be divided into two subcategories, the linkage isomers and coordination-sphere isomers.
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Isomers are different chemical species that have the same chemical formula.
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The alkali metal sodium (atomic number 11) has one more electron than the neon atom. This electron must go into the lowest-energy subshell available, the 3s orbital, giving a 1s22s22p63s1 configuration. The electrons occupying the outermost shell orbital(s) (highest value of n) are called valence electrons, and those occupying the inner shell orbitals are called core electrons. Since the core electron shells correspond to noble gas electron configurations, we can abbreviate electron...
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Accessing Valuable Ligand Supports for Transition Metals: A Modified, Intermediate Scale Preparation of 1,2,3,4,5-Pentamethylcyclopentadiene
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Cerio ((IV) Complejos de Imido: Estudios estructurales, computacionales y de reactividad

Lukman A Solola1, Alexander V Zabula1, Walter L Dorfner1

  • 1P. Roy and Diana T. Vagelos Laboratories, Department of Chemistry, University of Pennsylvania , 231 South 34th Street, Philadelphia, Pennsylvania 19104, United States.

Journal of the American Chemical Society
|January 13, 2017
PubMed
Resumen
Este resumen es generado por máquina.

Los cationes de metal alcalino influyen en la geometría compleja del cerio (IV), acortando el enlace CeN con el aumento del tamaño del cation. Se logró un nuevo enlace CeN sin soporte, con DFT revelando contribuciones orbitales 5d al enlace.

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Área de la Ciencia:

  • Química inorgánica
  • Química organometálica
  • Ciencias de los materiales

Sus antecedentes:

  • Los complejos de imido de cerio son de interés debido a su unión y reactividad únicas.
  • Comprender la influencia de los contraiones de metales alcalinos en estos complejos es crucial para el diseño de nuevos materiales y catalizadores.

Objetivo del estudio:

  • Para sintetizar y caracterizar una serie de metales alcalinos cubiertos de cerio (IV) complejos imido.
  • Investigar el impacto estructural de los contraiones de metales alcalinos en el enlace cerio-nitrógeno.
  • Para explorar la reactividad de estos nuevos complejos de cerio.

Principales métodos:

  • Síntesis y caracterización completa de los complejos de imido de cerio con capa de metal alcalino.
  • Investigación estructural de rayos X para determinar el impacto de los contraiones en la geometría compleja.
  • Cálculos de la Teoría Funcional de Densidad (DFT) para aclarar la estructura electrónica y el enlace.
  • Estudios de reactividad que incluyen la escisión de enlaces silicio-oxígeno y reacciones con benzofenona.

Principales resultados:

  • Aislamiento y caracterización de los complejos [M(solv) x][CeN(3,5-(CF3) 2C6H3) (M = Li, K, Rb, Cs).
  • Se observó un acortamiento del enlace CeN con un aumento del tamaño del catión de metal alcalino.
  • Aislamiento del primer complejo de enlaces múltiples Ce(IV) N no soportado con un contraion Cs+ y un criptando 2.2.2, con una longitud de enlace CeN de 2.077(3) Å.
  • Los estudios de DFT indicaron una contribución significativa del orbital de cerio 5d a los enlaces CeN.
  • Reactividad demostrada, incluida la escisión del enlace Si-O por un complejo de potasio y la formación de un complejo raro de Ce (IV) -oxo a partir de un complejo de rubidio.

Conclusiones:

  • Los contraiones de metales alcalinos juegan un papel importante en el ajuste de la estructura y el enlace de los complejos de cerio (IV) imido.
  • La capacidad de formar enlaces terminales Ce ((IV) N sin soporte abre nuevas vías en la química del cerio.
  • Estos complejos exhiben una reactividad interesante, destacando sus aplicaciones potenciales en catálisis y ciencia de materiales.