Yang, T., Ding, K., Zhou, J., Ma, X., Tan, K. C., Wang, G., Huang, H., & Yang, M. (2024). Unravelling Species‐Specific Loading Effects on Oxygen Reduction Activity of Heteronuclear Single Atom Catalysts. Small Methods, 9(5). Portico. https://doi.org/10.1002/smtd.202401333
Abstract:
AbstractToward high‐density single atom catalysts (SACs), the interaction between neighboring SACs and the induced non‐linear loading effect become crucial for their intrinsic catalytic performance. Despite recent investigations on homonuclear SACs, understanding such effect in heteronuclear SACs remains limited. Using Fe and Co SACs co‐supported on the nitrogen‐doped graphene as a model system, the loading effect on the site‐specific activity of heteronuclear SACs toward oxygen reduction reaction (ORR) is here reported by density functional theory calculations. The Fe site exhibits an oscillatory decrease in activity with the loading. In contrast, the Co site has a volcano‐like activity with the optimum performance achieved at ≈16.8 wt.% (average inter‐site distance: ≈7 Å). At the ultra‐high loading of 38.4 wt.% (inter‐site distance: ≈4 Å), the Co site is the only ORR active site, whereas Fe sites turn into spectators. This distinct loading‐dependent activity between the Fe and Co sites can be ascribed to their difference in the binding capability with the substrate and the dxz and dyz orbitals’ occupation. These findings highlight the importance of the loading effect in heteronuclear SACs, which could be useful for the development of high‐performance heteronuclear and high‐entropy SACs toward various catalytic reactions in the high‐loading regime.
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Description:
This is the peer reviewed version of the following article: Yang, T., Ding, K., Zhou, J., Ma, X., Tan, K. C., Wang, G., Huang, H., & Yang, M. (2024). Unravelling Species‐Specific Loading Effects on Oxygen Reduction Activity of Heteronuclear Single Atom Catalysts. Small Methods, 9(5). Portico. https://doi.org/10.1002/smtd.202401333 which has been published in final form athttps://doi.org/10.1002/smtd.202401333 . This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.