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Adsorption Device Based on a Langatate Crystal Microbalance for High Temperature High Pressure Gas Adsorption in Zeolite H-ZSM-5
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Sitios activos inducidos por el adsorbado en materiales de zeotipo
Guangchao Li1,2,3, Christopher Foo2,4, Xianfeng Yi1
1State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, People's Republic of China.
Journal of the American Chemical Society
|June 2, 2021
Resumen
Los investigadores observaron por primera vez sitios activos inducidos en materiales de silicoaluminophosphate (SAPO). Esto desafía la visión tradicional de los sitios activos fijos en las zeolitas, revelando la creación de sitios dinámicos durante la adsorción molecular y la catálisis.
Área de la Ciencia:
- Ciencias de los materiales
- Catálisis
- Química del estado sólido
Sus antecedentes:
- Las zeolitas son cruciales para aplicaciones industriales, con sitios activos tradicionalmente considerados fijos.
- La creación dinámica de sitios activos por adsorbados en materiales de zeotipo es en gran medida inexplorada.
- Los sitios ácidos de Lewis (LAS) y los sitios básicos de Lewis (LBS) son sitios activos aceptados en zeolitas prístinas.
Objetivo del estudio:
- Observar experimentalmente el establecimiento de sitios activos inducidos en silicoaluminophosphate (SAPO) por los adsorbados.
- Desafiar la comprensión convencional de los sitios activos fijos en los materiales de zeotipo.
- Investigar las interacciones dinámicas entre los adsorbados y los marcos de zeotipos.
Principales métodos:
- RMN de estado sólido de ángulo mágico de alta resolución
- Difracción de rayos X sincrotrón
- Difracción de polvo de neutrones
- Espectroscopia de la transformación de Fourier en el infrarrojo de reflectancia difusa in situ
- Dinámica molecular desde el principio
Principales resultados:
- Se obtuvieron pruebas experimentales directas de sitios activos inducidos en SAPO por adsorbados.
- Se observó una transformación de los sitios de ácido de Brønsted (Al ((OH) Si) a estructuras de par de Lewis frustradas inducidas (FLP).
- Las FLP inducidas, que comprenden tres estructuras coordinadas Al (LAS) y SiOH (LBS), favorecen transitoriamente la unión molecular heterolítica.
Conclusiones:
- El estudio demuestra el establecimiento dinámico de sitios activos en materiales de zeotipo.
- Los sitios activos inducidos pueden ser creados por bombardeo molecular, desafiando el paradigma del sitio fijo.
- Este hallazgo abre nuevas vías para comprender la adsorción y la catálisis en estructuras zeolíticas.
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