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Spin-related symmetry breaking induced by half-disordered hybridization in Bi(x)Er(2-x)Ru(2)O(7) pyrochlores for acidic oxygen evolution
While acidic oxygen evolution reaction plays a critical role in electrochemical energy conversion devices, the sluggish reaction kinetics and poor stability in acidic electrolyte challenges materials development. Unlike traditional nano-structuring approaches, this work focuses on the structural sym...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9287408/ https://www.ncbi.nlm.nih.gov/pubmed/35840581 http://dx.doi.org/10.1038/s41467-022-31874-4 |
Sumario: | While acidic oxygen evolution reaction plays a critical role in electrochemical energy conversion devices, the sluggish reaction kinetics and poor stability in acidic electrolyte challenges materials development. Unlike traditional nano-structuring approaches, this work focuses on the structural symmetry breaking to rearrange spin electron occupation and optimize spin-dependent orbital interaction to alter charge transfer between catalysts and reactants. Herein, we propose an atomic half-disordering strategy in multistage-hybridized Bi(x)Er(2-x)Ru(2)O(7) pyrochlores to reconfigure orbital degeneracy and spin-related electron occupation. This strategy involves controlling the bonding interaction of Bi-6s lone pair electrons, in which partial atom rearrangement makes the active sites transform into asymmetric high-spin states from symmetric low-spin states. As a result, the half-disordered Bi(x)Er(2-x)Ru(2)O(7) pyrochlores demonstrate an overpotential of ~0.18 V at 10 mA cm(−2) accompanied with excellent stability of 100 h in acidic electrolyte. Our findings not only provide a strategy for designing atom-disorder-related catalysts, but also provides a deeper understanding of the spin-related acidic oxygen evolution reaction kinetics. |
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