Rapid Surface Reconstruction of Pentlandite by High-Spin State Iron for Efficient Oxygen Evolution Reaction.
Angew Chem Int Ed Engl
; 63(6): e202317022, 2024 Feb 05.
Article
en En
| MEDLINE
| ID: mdl-38151463
ABSTRACT
Triggering rapid reconstruction reactions holds the potential to approach the theoretical limits of the oxygen evolution reaction (OER), and spin state manipulation has shown great promise in this regard. In this study, the transition of Fe spin states from low to high was successfully achieved by adjusting the surface electronic structure of pentlandite. In situ characterization and kinetic simulations confirmed that the high-spin state of Fe promoted the accumulation of OH- on the surface and accelerated electron transfer, thereby enhancing the kinetics of the reconstruction reaction. Furthermore, theoretical calculations revealed that the lower d-band center of high-spin Fe optimized the adsorption of active intermediates, thereby enhancing the reconstruction kinetics. Remarkably, pentlandites with high-spin Fe exhibited ultra-low overpotential (245â
mV @ 10â
mA cm-2 ) and excellent stability. These findings provided new insights for the design and fabrication of highly active OER electrocatalysts.
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1
Colección:
01-internacional
Banco de datos:
MEDLINE
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Año:
2024
Tipo del documento:
Article
País de afiliación:
China