Accelerated Anti‐Markovnikov Alkene Hydrosilylation with Humic‐Acid‐Supported Electron‐Deficient Platinum Single Atoms
| Autor: | Markus Antonietti, Bolortuya Badamdorj, Fan Yang, Michael J. Janik, Kairui Liu |
|---|---|
| Rok vydání: | 2021 |
| Předmět: |
chemistry.chemical_classification
artificial humic acid Alkene Hydrosilylation Inorganic chemistry Markovnikov's rule hydrosilylation chemistry.chemical_element Homogeneous catalysis General Medicine Pt single atom urea General Chemistry Electron deficiency Heterogeneous catalysis Catalysis chemistry.chemical_compound Heterogeneous Catalysis chemistry Platinum Research Articles Research Article |
| Zdroj: | Angewandte Chemie (International Ed. in English) Angewandte Chemie International Edition Angewandte Chemie |
| ISSN: | 1521-3773 1433-7851 |
| DOI: | 10.1002/anie.202109689 |
| Popis: | The hydrosilylation reaction is one of the largest‐scale applications of homogeneous catalysis, and Pt homogeneous catalysts have been widely used in this reaction for the commercial manufacture of silicon products. However, homogeneous Pt catalysts result in considerable problems, such as undesired side reactions, unacceptable catalyst residues and disposable platinum consumption. Here, we synthesized electron‐deficient Pt single atoms supported on humic matter (Pt1@AHA_U_400), and the catalyst was used in hydrosilylation reactions, which showed super activity (turnover frequency as high as 3.0×107 h−1) and selectivity (>99 %). Density functional theory calculations reveal that the high performance of the catalyst results from the atomic dispersion of Pt and the electron deficiency of the Pt1 atoms, which is different from conventional Pt nanoscale catalysts. Excellent performance is maintained during recycle experiments, indicating the high stability of the catalyst. A humic‐acid‐based carbonaceous support material AHA_U_400 was prepared through mild thermal condensation and cross‐linking between artificial humic acid and urea, and the material proved to enable the preparation of the stable Pt single‐atom catalyst (Pt1@AHA_U_400). Pt was coordinated to two unsaturated O atoms, as well as one Cl− and one HCl moiety. |
| Databáze: | OpenAIRE |
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