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DC Field | Value | Language |
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dc.citation.number | 20 | - |
dc.citation.startPage | e202403017 | - |
dc.citation.title | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | - |
dc.citation.volume | 63 | - |
dc.contributor.author | Che, Wei | - |
dc.contributor.author | Li, Pai | - |
dc.contributor.author | Han, Gao-Feng | - |
dc.contributor.author | Noh, Hyuk-Jun | - |
dc.contributor.author | Seo, Jeong-Min | - |
dc.contributor.author | Jeon, Jong-Pil | - |
dc.contributor.author | Li, Changqing | - |
dc.contributor.author | Liu, Wei | - |
dc.contributor.author | Li, Feng | - |
dc.contributor.author | Liu, Qinghua | - |
dc.contributor.author | Baek, Jong-Beom | - |
dc.date.accessioned | 2024-04-15T09:35:11Z | - |
dc.date.available | 2024-04-15T09:35:11Z | - |
dc.date.created | 2024-04-09 | - |
dc.date.issued | 2024-05 | - |
dc.description.abstract | Crafting single-atom catalysts (SACs) that possess "just right" modulated electronic and geometric structures, granting accessible active sites for direct room-temperature benzene oxidation is a coveted objective. However, achieving this goal remains a formidable challenge. Here, we introduce an innovative in situ phosphorus-immitting strategy using a new phosphorus source (phosphorus nitride, P3N5) to construct the phosphorus-rich copper (Cu) SACs, designated as Cu/NPC. These catalysts feature locally protruding metal sites on a nitrogen (N)-phosphorus (P)-carbon (C) support (NPC). Rigorous analyses, including X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectroscopy (XPS), validate the coordinated bonding of nitrogen and phosphorus with atomically dispersed Cu sites on NPC. Crucially, systematic first-principles calculations, coupled with the climbing image nudged-elastic-band (CI-NEB) method, provide a comprehensive understanding of the structure-property-activity relationship of the distorted Cu-N2P2 centers in Cu/NPC for selective oxidation of benzene to phenol production. Interestingly, Cu/NPC has shown more energetically favorable C-H bond activation compared to the benchmark Cu/NC SACs in the direct oxidation of benzene, resulting in outstanding benzene conversion (50.3 %) and phenol selectivity (99.3 %) at room temperature. Furthermore, Cu/NPC achieves a remarkable turnover frequency of 263 h-1 and mass-specific activity of 35.2 mmol g-1 h-1, surpassing the state-of-the-art benzene-to-phenol conversion catalysts to date. Copper single-atom catalysts (Cu SACs, designated as Cu/NPC) with the out-of-plane Cu sites on the nitrogen (N)-phosphorus (P)-carbon (C) support were synthesized using an in situ phosphorous-immitting method. The P-rich coordinated Cu sites of the Cu/NPC were responsible for the direct C-H activation of benzene to phenol conversion.+ image | - |
dc.identifier.bibliographicCitation | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, v.63, no.20, pp.e202403017 | - |
dc.identifier.doi | 10.1002/anie.202403017 | - |
dc.identifier.issn | 1433-7851 | - |
dc.identifier.scopusid | 2-s2.0-85187945634 | - |
dc.identifier.uri | https://scholarworks.unist.ac.kr/handle/201301/82250 | - |
dc.identifier.wosid | 001187042300001 | - |
dc.language | 영어 | - |
dc.publisher | WILEY-V C H VERLAG GMBH | - |
dc.title | Out-of-Plane Single-Copper-Site Catalysts for Room-Temperature Benzene Oxidation | - |
dc.type | Article | - |
dc.description.isOpenAccess | FALSE | - |
dc.relation.journalWebOfScienceCategory | Chemistry, Multidisciplinary | - |
dc.relation.journalResearchArea | Chemistry | - |
dc.type.docType | Article; Early Access | - |
dc.description.journalRegisteredClass | scie | - |
dc.description.journalRegisteredClass | scopus | - |
dc.subject.keywordAuthor | benzene hydroxylation | - |
dc.subject.keywordAuthor | electron localization | - |
dc.subject.keywordAuthor | geometric feature | - |
dc.subject.keywordAuthor | green chemistry | - |
dc.subject.keywordAuthor | single-atom catalysts | - |
dc.subject.keywordPlus | OXYGEN REDUCTION | - |
dc.subject.keywordPlus | HYDROGEN-PEROXIDE | - |
dc.subject.keywordPlus | CARBON | - |
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