Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition
Abstract Modulation of electronic spin states in cobalt-based catalysts is an effective strategy for molecule activations. Crystalline-amorphous interfaces often exhibit unique catalytic properties due to disruptions of long-range order and alterations in electronic structure. However, the mechanism...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56487-5 |
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| author | Yunpeng Long Xiao Zhu Chuan Gao Wenzhe Si Junhua Li Yue Peng |
| author_facet | Yunpeng Long Xiao Zhu Chuan Gao Wenzhe Si Junhua Li Yue Peng |
| author_sort | Yunpeng Long |
| collection | DOAJ |
| description | Abstract Modulation of electronic spin states in cobalt-based catalysts is an effective strategy for molecule activations. Crystalline-amorphous interfaces often exhibit unique catalytic properties due to disruptions of long-range order and alterations in electronic structure. However, the mechanisms of molecule activation and spin states at interfaces remain elusive. Herein, we present a Co3O4 spinel-based catalyst featuring crystalline-amorphous interfaces. Characterization analyses confirm that tetrahedral Co2+ is selectively etched from bulk spinel, forming amorphous CoO islands on the surface. The resultant symmetry breaking in the coordination field induces a reconstruction of the Co3+ 3 d orbitals, leading to high-spin states. In CO oxidation, the interface serves as novel active sites with a lower energy barrier, facilitated by lattice oxygen activation. In N2O decomposition, the interface promotes reassociation of dissociated oxygen through quantum spin exchange interactions. This work provides a straightforward approach to modulating the spin state of interfaces and elucidates their role in molecule activations. |
| format | Article |
| id | doaj-art-09a34f0297a54ad49b0b4a7dcd67b7b1 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-09a34f0297a54ad49b0b4a7dcd67b7b12025-01-26T12:42:26ZengNature PortfolioNature Communications2041-17232025-01-0116111110.1038/s41467-025-56487-5Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decompositionYunpeng Long0Xiao Zhu1Chuan Gao2Wenzhe Si3Junhua Li4Yue Peng5School of Environment, Tsinghua UniversitySchool of Environment, Tsinghua UniversitySchool of Environment, Tsinghua UniversitySchool of Environment, Tsinghua UniversitySchool of Environment, Tsinghua UniversitySchool of Environment, Tsinghua UniversityAbstract Modulation of electronic spin states in cobalt-based catalysts is an effective strategy for molecule activations. Crystalline-amorphous interfaces often exhibit unique catalytic properties due to disruptions of long-range order and alterations in electronic structure. However, the mechanisms of molecule activation and spin states at interfaces remain elusive. Herein, we present a Co3O4 spinel-based catalyst featuring crystalline-amorphous interfaces. Characterization analyses confirm that tetrahedral Co2+ is selectively etched from bulk spinel, forming amorphous CoO islands on the surface. The resultant symmetry breaking in the coordination field induces a reconstruction of the Co3+ 3 d orbitals, leading to high-spin states. In CO oxidation, the interface serves as novel active sites with a lower energy barrier, facilitated by lattice oxygen activation. In N2O decomposition, the interface promotes reassociation of dissociated oxygen through quantum spin exchange interactions. This work provides a straightforward approach to modulating the spin state of interfaces and elucidates their role in molecule activations.https://doi.org/10.1038/s41467-025-56487-5 |
| spellingShingle | Yunpeng Long Xiao Zhu Chuan Gao Wenzhe Si Junhua Li Yue Peng Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition Nature Communications |
| title | Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition |
| title_full | Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition |
| title_fullStr | Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition |
| title_full_unstemmed | Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition |
| title_short | Modulation of Co spin state at Co3O4 crystalline-amorphous interfaces for CO oxidation and N2O decomposition |
| title_sort | modulation of co spin state at co3o4 crystalline amorphous interfaces for co oxidation and n2o decomposition |
| url | https://doi.org/10.1038/s41467-025-56487-5 |
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