Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions
Abstract In this study, we introduce a highly effective non-metallic iodine single-atom catalyst (SAC), referred to as I-NC, which is strategically confined within a nitrogen-doped carbon (NC) scaffold. This configuration features a distinctive C-I coordination that optimizes the electronic structur...
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56246-6 |
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| author | Junjun Pei Jianbin Liu Kaixing Fu Yukui Fu Kai Yin Shenglian Luo Deyou Yu Mingyang Xing Jinming Luo |
| author_facet | Junjun Pei Jianbin Liu Kaixing Fu Yukui Fu Kai Yin Shenglian Luo Deyou Yu Mingyang Xing Jinming Luo |
| author_sort | Junjun Pei |
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| description | Abstract In this study, we introduce a highly effective non-metallic iodine single-atom catalyst (SAC), referred to as I-NC, which is strategically confined within a nitrogen-doped carbon (NC) scaffold. This configuration features a distinctive C-I coordination that optimizes the electronic structure of the nitrogen-adjacent carbon sites. As a result, this arrangement enhances electron transfer from peroxymonosulfate (PMS) to the active sites, particularly the electron-deficient carbon. This electron transfer is followed by a deprotonation process that generates the peroxymonosulfate radical (SO5 •−). Subsequently, the SO5 •− radical undergoes a disproportionation reaction, leading to the production of singlet oxygen (1O2). Furthermore, the energy barrier for the rate-limiting step of SO5 •− generation in I-NC is significantly lower at 1.45 eV, compared to 1.65 eV in the NC scaffold. This reduction in energy barrier effectively overcomes kinetic obstacles, thereby facilitating an enhanced generation of 1O2. Consequently, the I-NC catalyst exhibits remarkable catalytic efficiency and unmatched reactivity for PMS activation. This leads to a significantly accelerated degradation of pollutants, evidenced by a relatively high observed kinetic rate constant (k obs ~ 0.436 min− 1) compared to other metallic SACs. This study offers valuable insights into the rational design of effective non-metallic SACs, showcasing their promising potential for Fenton-like reactions in water treatment applications. |
| format | Article |
| id | doaj-art-005b7d2dc090490e97f53788b4d7b647 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
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| spelling | doaj-art-005b7d2dc090490e97f53788b4d7b6472025-01-19T12:31:20ZengNature PortfolioNature Communications2041-17232025-01-0116111210.1038/s41467-025-56246-6Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactionsJunjun Pei0Jianbin Liu1Kaixing Fu2Yukui Fu3Kai Yin4Shenglian Luo5Deyou Yu6Mingyang Xing7Jinming Luo8College of Environmental Science and Engineering, Hunan UniversityState Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan UniversityState Environmental Protection Key Laboratory of Environmental Health Impact Assessment of Emerging Contaminants, School of Environmental Science and Engineering, Shanghai Jiao Tong UniversityCollege of Environmental Science and Engineering, Hunan UniversityCollege of Environmental Science and Engineering, Hunan UniversityCollege of Environmental Science and Engineering, Hunan UniversityEngineering Research Center for Eco-Dyeing and Finishing of Textiles (Ministry of Education), Zhejiang Sci-Tech UniversitySchool of Chemistry and Molecular Engineering, East China University of Science and TechnologyState Environmental Protection Key Laboratory of Environmental Health Impact Assessment of Emerging Contaminants, School of Environmental Science and Engineering, Shanghai Jiao Tong UniversityAbstract In this study, we introduce a highly effective non-metallic iodine single-atom catalyst (SAC), referred to as I-NC, which is strategically confined within a nitrogen-doped carbon (NC) scaffold. This configuration features a distinctive C-I coordination that optimizes the electronic structure of the nitrogen-adjacent carbon sites. As a result, this arrangement enhances electron transfer from peroxymonosulfate (PMS) to the active sites, particularly the electron-deficient carbon. This electron transfer is followed by a deprotonation process that generates the peroxymonosulfate radical (SO5 •−). Subsequently, the SO5 •− radical undergoes a disproportionation reaction, leading to the production of singlet oxygen (1O2). Furthermore, the energy barrier for the rate-limiting step of SO5 •− generation in I-NC is significantly lower at 1.45 eV, compared to 1.65 eV in the NC scaffold. This reduction in energy barrier effectively overcomes kinetic obstacles, thereby facilitating an enhanced generation of 1O2. Consequently, the I-NC catalyst exhibits remarkable catalytic efficiency and unmatched reactivity for PMS activation. This leads to a significantly accelerated degradation of pollutants, evidenced by a relatively high observed kinetic rate constant (k obs ~ 0.436 min− 1) compared to other metallic SACs. This study offers valuable insights into the rational design of effective non-metallic SACs, showcasing their promising potential for Fenton-like reactions in water treatment applications.https://doi.org/10.1038/s41467-025-56246-6 |
| spellingShingle | Junjun Pei Jianbin Liu Kaixing Fu Yukui Fu Kai Yin Shenglian Luo Deyou Yu Mingyang Xing Jinming Luo Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions Nature Communications |
| title | Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions |
| title_full | Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions |
| title_fullStr | Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions |
| title_full_unstemmed | Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions |
| title_short | Non-metallic iodine single-atom catalysts with optimized electronic structures for efficient Fenton-like reactions |
| title_sort | non metallic iodine single atom catalysts with optimized electronic structures for efficient fenton like reactions |
| url | https://doi.org/10.1038/s41467-025-56246-6 |
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