Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis
Abstract The tunability of reaction pathways is required for exploring efficient and low cost catalysts for ammonia synthesis. There is an obstacle by the limitations arising from scaling relation for this purpose. Here, we demonstrate that the alkali earth imides (AeNH) combined with transition met...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-10-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-42050-7 |
| _version_ | 1797557925486526464 |
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| author | Zichuang Li Yangfan Lu Jiang Li Miao Xu Yanpeng Qi Sang-Won Park Masaaki Kitano Hideo Hosono Jie-Sheng Chen Tian-Nan Ye |
| author_facet | Zichuang Li Yangfan Lu Jiang Li Miao Xu Yanpeng Qi Sang-Won Park Masaaki Kitano Hideo Hosono Jie-Sheng Chen Tian-Nan Ye |
| author_sort | Zichuang Li |
| collection | DOAJ |
| description | Abstract The tunability of reaction pathways is required for exploring efficient and low cost catalysts for ammonia synthesis. There is an obstacle by the limitations arising from scaling relation for this purpose. Here, we demonstrate that the alkali earth imides (AeNH) combined with transition metal (TM = Fe, Co and Ni) catalysts can overcome this difficulty by utilizing functionalities arising from concerted role of active defects on the support surface and loaded transition metals. These catalysts enable ammonia production through multiple reaction pathways. The reaction rate of Co/SrNH is as high as 1686.7 mmol·gCo −1·h−1 and the TOFs reaches above 500 h−1 at 400 °C and 0.9 MPa, outperforming other reported Co-based catalysts as well as the benchmark Cs-Ru/MgO catalyst and industrial wüstite-based Fe catalyst under the same reaction conditions. Experimental and theoretical results show that the synergistic effect of nitrogen affinity of 3d TMs and in-situ formed NH2− vacancy of alkali earth imides regulate the reaction pathways of the ammonia production, resulting in distinct catalytic performance different from 3d TMs. It was thus demonstrated that the appropriate combination of metal and support is essential for controlling the reaction pathway and realizing highly active and low cost catalysts for ammonia synthesis. |
| first_indexed | 2024-03-10T17:24:08Z |
| format | Article |
| id | doaj.art-24085b026b7044a5b79f499a478536ed |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-10T17:24:08Z |
| publishDate | 2023-10-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-24085b026b7044a5b79f499a478536ed2023-11-20T10:14:13ZengNature PortfolioNature Communications2041-17232023-10-0114111210.1038/s41467-023-42050-7Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesisZichuang Li0Yangfan Lu1Jiang Li2Miao Xu3Yanpeng Qi4Sang-Won Park5Masaaki Kitano6Hideo Hosono7Jie-Sheng Chen8Tian-Nan Ye9Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong UniversityCollege of Materials Science and Engineering, National Engineering Research Center for Magnesium Alloys, Chongqing UniversityMaterials Research Center for Element Strategy, Tokyo Institute of TechnologyState Key Laboratory of Space Power Sources, Shanghai Institute of Space Power-SourcesSchool of Physical Science and Technology Shanghai Tech UniversityMaterials Research Center for Element Strategy, Tokyo Institute of TechnologyMaterials Research Center for Element Strategy, Tokyo Institute of TechnologyMaterials Research Center for Element Strategy, Tokyo Institute of TechnologyFrontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong UniversityFrontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong UniversityAbstract The tunability of reaction pathways is required for exploring efficient and low cost catalysts for ammonia synthesis. There is an obstacle by the limitations arising from scaling relation for this purpose. Here, we demonstrate that the alkali earth imides (AeNH) combined with transition metal (TM = Fe, Co and Ni) catalysts can overcome this difficulty by utilizing functionalities arising from concerted role of active defects on the support surface and loaded transition metals. These catalysts enable ammonia production through multiple reaction pathways. The reaction rate of Co/SrNH is as high as 1686.7 mmol·gCo −1·h−1 and the TOFs reaches above 500 h−1 at 400 °C and 0.9 MPa, outperforming other reported Co-based catalysts as well as the benchmark Cs-Ru/MgO catalyst and industrial wüstite-based Fe catalyst under the same reaction conditions. Experimental and theoretical results show that the synergistic effect of nitrogen affinity of 3d TMs and in-situ formed NH2− vacancy of alkali earth imides regulate the reaction pathways of the ammonia production, resulting in distinct catalytic performance different from 3d TMs. It was thus demonstrated that the appropriate combination of metal and support is essential for controlling the reaction pathway and realizing highly active and low cost catalysts for ammonia synthesis.https://doi.org/10.1038/s41467-023-42050-7 |
| spellingShingle | Zichuang Li Yangfan Lu Jiang Li Miao Xu Yanpeng Qi Sang-Won Park Masaaki Kitano Hideo Hosono Jie-Sheng Chen Tian-Nan Ye Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis Nature Communications |
| title | Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis |
| title_full | Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis |
| title_fullStr | Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis |
| title_full_unstemmed | Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis |
| title_short | Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis |
| title_sort | multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis |
| url | https://doi.org/10.1038/s41467-023-42050-7 |
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