Effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decomposition
Abstract Nitrogen-containing compounds such as imides and amides have been reported as efficient materials that promote ammonia decomposition over nonnoble metal catalysts. However, these compounds decompose in an air atmosphere and become inactive, which leads to difficulty in handling. Here, we fo...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-10-01
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| Series: | NPG Asia Materials |
| Online Access: | https://doi.org/10.1038/s41427-024-00572-6 |
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| author | Kazuki Miyashita Kiya Ogasawara Masayoshi Miyazaki Hitoshi Abe Yasuhiro Niwa Hideki Kato Hideo Hosono Masaaki Kitano |
| author_facet | Kazuki Miyashita Kiya Ogasawara Masayoshi Miyazaki Hitoshi Abe Yasuhiro Niwa Hideki Kato Hideo Hosono Masaaki Kitano |
| author_sort | Kazuki Miyashita |
| collection | DOAJ |
| description | Abstract Nitrogen-containing compounds such as imides and amides have been reported as efficient materials that promote ammonia decomposition over nonnoble metal catalysts. However, these compounds decompose in an air atmosphere and become inactive, which leads to difficulty in handling. Here, we focused on perovskite oxynitrides as air-stable and efficient supports for ammonia decomposition catalysts. Ni-loaded oxynitrides exhibited 2.5–18 times greater catalytic activity than did the corresponding oxide-supported Ni catalysts, even without noticeable differences in the Ni particle size and surface area of the supports. The catalytic performance of the Ni-loaded oxynitrides is well correlated with the nitrogen desorption temperature during N2 temperature-programmed desorption, which suggests that the lattice nitrogen in the oxynitride support rather than the Ni surface is the active site for ammonia decomposition. Furthermore, NH3 temperature-programmed surface reactions and density functional theory (DFT) calculations revealed that NH3 molecules are preferentially adsorbed on the nitrogen vacancy sites on the support surface rather than on the Ni surface. Thus, the ammonia decomposition reaction is facilitated by a vacancy-mediated reaction mechanism. |
| format | Article |
| id | doaj-art-e1920a685cd74455ab5bd40bed4085b6 |
| institution | Kabale University |
| issn | 1884-4057 |
| language | English |
| publishDate | 2024-10-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | NPG Asia Materials |
| spelling | doaj-art-e1920a685cd74455ab5bd40bed4085b62025-01-19T12:29:01ZengNature PortfolioNPG Asia Materials1884-40572024-10-011611910.1038/s41427-024-00572-6Effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decompositionKazuki Miyashita0Kiya Ogasawara1Masayoshi Miyazaki2Hitoshi Abe3Yasuhiro Niwa4Hideki Kato5Hideo Hosono6Masaaki Kitano7MDX Research Center for Element Strategy, International Research Frontiers Initiative, Tokyo Institute of TechnologyMDX Research Center for Element Strategy, International Research Frontiers Initiative, Tokyo Institute of TechnologyMDX Research Center for Element Strategy, International Research Frontiers Initiative, Tokyo Institute of TechnologyInstitute of Materials Structure Science, High Energy Accelerator Research OrganizationInstitute of Materials Structure Science, High Energy Accelerator Research OrganizationInstitute of Multidisciplinary Research for Advanced Materials, Tohoku UniversityMDX Research Center for Element Strategy, International Research Frontiers Initiative, Tokyo Institute of TechnologyMDX Research Center for Element Strategy, International Research Frontiers Initiative, Tokyo Institute of TechnologyAbstract Nitrogen-containing compounds such as imides and amides have been reported as efficient materials that promote ammonia decomposition over nonnoble metal catalysts. However, these compounds decompose in an air atmosphere and become inactive, which leads to difficulty in handling. Here, we focused on perovskite oxynitrides as air-stable and efficient supports for ammonia decomposition catalysts. Ni-loaded oxynitrides exhibited 2.5–18 times greater catalytic activity than did the corresponding oxide-supported Ni catalysts, even without noticeable differences in the Ni particle size and surface area of the supports. The catalytic performance of the Ni-loaded oxynitrides is well correlated with the nitrogen desorption temperature during N2 temperature-programmed desorption, which suggests that the lattice nitrogen in the oxynitride support rather than the Ni surface is the active site for ammonia decomposition. Furthermore, NH3 temperature-programmed surface reactions and density functional theory (DFT) calculations revealed that NH3 molecules are preferentially adsorbed on the nitrogen vacancy sites on the support surface rather than on the Ni surface. Thus, the ammonia decomposition reaction is facilitated by a vacancy-mediated reaction mechanism.https://doi.org/10.1038/s41427-024-00572-6 |
| spellingShingle | Kazuki Miyashita Kiya Ogasawara Masayoshi Miyazaki Hitoshi Abe Yasuhiro Niwa Hideki Kato Hideo Hosono Masaaki Kitano Effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decomposition NPG Asia Materials |
| title | Effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decomposition |
| title_full | Effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decomposition |
| title_fullStr | Effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decomposition |
| title_full_unstemmed | Effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decomposition |
| title_short | Effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decomposition |
| title_sort | effects of nitrogen vacancy sites of oxynitride support on the catalytic activity for ammonia decomposition |
| url | https://doi.org/10.1038/s41427-024-00572-6 |
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