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Los monoésteres de fosfonato como enlaces similares a los carboxilatos para estructuras orgánicas metálicas
Simon S Iremonger1, Junmei Liang, Ramanathan Vaidhyanathan
1Department of Chemistry, University of Calgary, Calgary T2N 1N4, Canada.
Journal of the American Chemical Society
|November 19, 2011
Resumen
Las nuevas estructuras metal-orgánicas (MOF) que utilizan enlaces de monoéster de fosfonato son prometedoras para la captura de dióxido de carbono. Un atado de metilo permite una estructura porosa con alta adsorción de CO2, a diferencia de su homólogo atado de etilo.
Área de la Ciencia:
- Ciencia de los materiales Ciencia de los materiales.
- Química Inorgánica La Química Inorgánica es la química inorgánica.
- Química supramolecular de las moléculas.
Sus antecedentes:
- Los monoésteres de fosfonato de bidentato son análogos estructurales de los enlaces dicarboxilatos comunes utilizados en las estructuras orgánicas metálicas (MOF).
- Estos enlaces cuentan con un algodón alcoxi colocado cerca del sitio de coordinación, lo que puede influir en las propiedades del marco.
Objetivo del estudio:
- Para sintetizar y caracterizar 3-D metal-estructura orgánica (MOF) materiales que utilizan enlaces de monoéster de fosfonato.
- Investigar el impacto de la longitud del alquilo en las propiedades estructurales y de adsorción de gases de estos MOF.
Principales métodos:
- Síntesis de Cu{1,4-benzenediphosphonate bis{monoalkyl ester)) (CuBDPR) en marcos con diferentes éteres de alquilo (metilo y etilo).
- Caracterización de las estructuras MOF resultantes utilizando difracción de rayos X y análisis de adsorción de gases.
- Modelado computacional para comprender los mecanismos de adsorción de CO2.
Principales resultados:
- Se descubrió que el marco CuBDPR atado al etilo no era poroso.
- El marco CuBDPR atado al metilo formó una estructura isomorfa y porosa.
- El MOF poroso atado al metilo demostró una capacidad significativa de captura de CO2 con un alto calor isostérico de adsorción (45 kJ mol(-1)).
- Los estudios computacionales indicaron una alta sensibilidad de la absorción de CO2 a la flexibilidad estructural y la orientación de la sujeción.
Conclusiones:
- La elección del éter de alquilo en los enlaces de monoéster de fosfonato influye críticamente en la porosidad y el rendimiento de adsorción de CO2 de los MOF.
- El CuBDPR atado al metilo representa un material prometedor para aplicaciones de captura de CO2.
- La dinámica estructural y la orientación del enlace son factores clave que rigen la absorción de gas en estos MOF.
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