Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides
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...
| Main Authors: | , , , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-44587-z |
| _version_ | 1797363117070483456 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Shengnan Sun |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-03-08T16:16:42Z |
| format | Article |
| id | doaj.art-c326e13d6dd745e19d97b316f6c59d66 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-08T16:16:42Z |
| publishDate | 2024-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-c326e13d6dd745e19d97b316f6c59d662024-01-07T12:34:33ZengNature PortfolioNature Communications2041-17232024-01-0115111310.1038/s41467-023-44587-zSpin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxidesShengnan Sun0Chencheng Dai1Peng Zhao2Shibo Xi3Yi Ren4Hui Ru Tan5Poh Chong Lim6Ming Lin7Caozheng Diao8Danwei Zhang9Chao Wu10Anke Yu11Jie Cheng Jackson Koh12Wei Ying Lieu13Debbie Hwee Leng Seng14Libo Sun15Yuke Li16Teck Leong Tan17Jia Zhang18Zhichuan J. Xu19Zhi Wei Seh20Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)School of Materials Science and Engineering, Nanyang Technological UniversityInstitute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR)Institute of Sustainability for Chemicals, Energy and Environment (ISCE²), Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Singapore Synchrotron Light Sources (SSLS), National University of Singapore, 5 Research LinkInstitute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Institute of Sustainability for Chemicals, Energy and Environment (ISCE²), Agency for Science, Technology and Research (A*STAR)School of Materials Science and Engineering, Nanyang Technological UniversitySchool of Materials Science and Engineering, Nanyang Technological UniversityInstitute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)The Cambridge Centre for Advanced Research and Education in SingaporeInstitute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR)Institute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR)Institute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR)School of Materials Science and Engineering, Nanyang Technological UniversityInstitute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR)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.https://doi.org/10.1038/s41467-023-44587-z |
| spellingShingle | 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 Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides Nature Communications |
| title | Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides |
| title_full | Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides |
| title_fullStr | Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides |
| title_full_unstemmed | Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides |
| title_short | Spin-related Cu-Co pair to increase electrochemical ammonia generation on high-entropy oxides |
| title_sort | spin related cu co pair to increase electrochemical ammonia generation on high entropy oxides |
| url | https://doi.org/10.1038/s41467-023-44587-z |
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