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

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 () and Zhi Wei Seh ()
Additional contact information
Shengnan Sun: Agency for Science, Technology and Research (A*STAR)
Chencheng Dai: Nanyang Technological University
Peng Zhao: Agency for Science, Technology and Research (A*STAR)
Shibo Xi: Energy and Environment (ISCE²), Agency for Science, Technology and Research (A*STAR)
Yi Ren: Agency for Science, Technology and Research (A*STAR)
Hui Ru Tan: Agency for Science, Technology and Research (A*STAR)
Poh Chong Lim: Agency for Science, Technology and Research (A*STAR)
Ming Lin: Agency for Science, Technology and Research (A*STAR)
Caozheng Diao: National University of Singapore, 5 Research Link
Danwei Zhang: Agency for Science, Technology and Research (A*STAR)
Chao Wu: Energy and Environment (ISCE²), Agency for Science, Technology and Research (A*STAR)
Anke Yu: Nanyang Technological University
Jie Cheng Jackson Koh: Nanyang Technological University
Wei Ying Lieu: Agency for Science, Technology and Research (A*STAR)
Debbie Hwee Leng Seng: Agency for Science, Technology and Research (A*STAR)
Libo Sun: The Cambridge Centre for Advanced Research and Education in Singapore
Yuke Li: Agency for Science, Technology and Research (A*STAR)
Teck Leong Tan: Agency for Science, Technology and Research (A*STAR)
Jia Zhang: Agency for Science, Technology and Research (A*STAR)
Zhichuan J. Xu: Nanyang Technological University
Zhi Wei Seh: Agency for Science, Technology and Research (A*STAR)

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract The 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.

Date: 2024
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DOI: 10.1038/s41467-023-44587-z

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