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Los entornos locales de litio reingresante y la electroquímica impulsada por defectos de los cátodos de las baterías
Fulya Dogan1, Brandon R Long, Jason R Croy
1Chemical Sciences and Engineering Division, ‡Materials Sciences Division, and §X-ray Science Division, Advanced Photon Source, Argonne National Laboratory , Argonne, Illinois 60439, United States.
Journal of the American Chemical Society
|January 31, 2015
Resumen
La investigación de óxidos en capas ricos en litio y manganeso utilizando (6) RMN giratoria de ángulo mágico de litio revela ocupación del sitio de litio dependiente de la ruta. Esta visión estructural explica la histeresis electroquímica y el impacto de las migraciones de metales de transición en las baterías secundarias.
Área de la Ciencia:
- Ciencia de los materiales Ciencia de los materiales.
- La electroquímica es electroquímica.
- Química del estado sólido.
Sus antecedentes:
- Comprender las relaciones estructura-actividad electroquímica es crucial para el desarrollo de baterías secundarias.
- La caracterización de los entornos locales de litio es clave para optimizar los materiales de intercalación.
- (6) La RMN Li MAS es una herramienta única para el análisis estructural a escala subnanométrica.
Objetivo del estudio:
- Investigar el complejo comportamiento electroquímico de los óxidos activados de metales de transición ricos en litio y manganeso.
- Para correlacionar la reorganización estructural con la histeresis electroquímica durante el ciclo.
- Para identificar y caracterizar sitios específicos de litio y su papel en el rendimiento de la batería.
Principales métodos:
- Utilizando la espectroscopia de resonancia magnética nuclear (RMN) de giro de ángulo mágico (MAS) (6) Li.
- Analizando los electrodos de intercalación de iones de litio (Li-ion) compuestos por 0.5(6) Li2MnO3·0.5(6) LiMn(0.5) Ni(0.5) O2.
- Observar los procesos de inserción y extracción de litio.
Principales resultados:
- Se observó evidencia directa de ocupación del sitio de litio dependiente del camino.
- Se identificaron nuevas (6) resonancias de RMN Li a ~ 1600 ppm asignadas a sitios LiMn6-TM(tet).
- Las migraciones TM reversibles, indicadas por la pérdida de sitios de litio en la capa TM, fueron limitadas durante el ciclo.
Conclusiones:
- La reorganización estructural y la ocupación de litio dependiente del camino se correlacionan directamente con la histeresis electroquímica.
- Los metales de transición tetraédricos (TM) reingresantes influyen en la ocupación del sitio del litio y en el comportamiento electroquímico.
- Incluso los sitios de defectos diluidos tienen un impacto significativo en el rendimiento electroquímico general de los materiales de intercalación de iones de litio.
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