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

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

Nature Communications

10.1038/s41467-023-44587-z

http://dx.doi.org/10.1038/s41467-023-44587-z

Shengnan Sun, Chencheng Dai, Peng Zhao, Shibo Xi, Yi Ren, Hui Ru Tan, Poh Chong Lim, Ming Lin, Caozheng Diao, Danwei Zhang, Chao Wu, Anke Yu, Jie Cheng Jackson Koh, Wei Ying Lieu, Debbie Hwee Leng Seng, Libo Sun, Yuke Li, Teck Leong Tan, Jia Zhang, Zhichuan J. Xu, Zhi Wei Seh

04 January 2024

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

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.

Attribution 4.0 International (CC BY 4.0)

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

https://oar.a-star.edu.sg/communities-collections/articles/20219

2041-1723

Institute of Materials Research & Engineering

https://doi.org/10.1038/s41467-023-44587-z