Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides

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Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides
Title:
Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides
Journal Title:
Nature Communications
Keywords:
Publication Date:
04 January 2024
Citation:
Sun, S., Dai, C., Zhao, P., Xi, S., Ren, Y., Tan, H. R., Lim, P. C., Lin, M., Diao, C., Zhang, D., Wu, C., Yu, A., Koh, J. C. J., Lieu, W. Y., Seng, D. H. L., Sun, L., Li, Y., Tan, T. L., Zhang, J., … Seh, Z. W. (2024). Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides. Nature Communications, 15(1). https://doi.org/10.1038/s41467-023-44587-z
Abstract:
AbstractThe electrochemical conversion of nitrate to ammonia is a way to eliminate nitrate pollutant in water. Cu-Co synergistic effect was found to produce excellent performance in ammonia generation. However, few studies have focused on this effect in high-entropy oxides. Here, we report the spin-related Cu-Co synergistic effect on electrochemical nitrate-to-ammonia conversion using high-entropy oxide Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O. In contrast, the Li-incorporated MgCoNiCuZnO exhibits inferior performance. By correlating the electronic structure, we found that the Co spin states are crucial for the Cu-Co synergistic effect for ammonia generation. The Cu-Co pair with a high spin Co in Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O can facilitate ammonia generation, while a low spin Co in Li-incorporated MgCoNiCuZnO decreases the Cu-Co synergistic effect on ammonia generation. These findings offer important insights in employing the synergistic effect and spin states inside for selective catalysis. It also indicates the generality of the magnetic effect in ammonia synthesis between electrocatalysis and thermal catalysis.
License type:
Attribution 4.0 International (CC BY 4.0)
Funding Info:
This research is supported by core funding from: SERC
Grant Reference no. : CRF

This research / project is supported by the A*STAR - AME IAF-PP
Grant Reference no. : A19E9a0103

This research / project is supported by the A*STAR - MTC Individual Research Grants (IRG)
Grant Reference no. : M22K2c0078

This research / project is supported by the National Research Foundation - Campus for Research Excellence and Technological Enterprise (CREATE) programme
Grant Reference no. : NA
Description:
ISSN:
2041-1723