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Metal‐Oxo Electronic Tuning via In Situ CO Decoration for Promoting Methane Conversion to Oxygenates over Single‐Atom Catalysts.
- Source :
-
Angewandte Chemie International Edition . Apr2024, Vol. 63 Issue 16, p1-7. 7p. - Publication Year :
- 2024
-
Abstract
- Direct methane conversion (DMC) to oxygenates at low temperature is of great value but remains challenging due to the high energy barrier for C−H bond activation. Here, we report that in situ decoration of Pd1‐ZSM‐5 single atom catalyst (SAC) by CO molecules significantly promoted the DMC reaction, giving the highest turnover frequency of 207 h−1 ever reported at room temperature and ~100 % oxygenates selectivity with H2O2 as oxidant. Combined characterizations and DFT calculations illustrate that the C‐atom of CO prefers to coordinate with Pd1, which donates electrons to the Pd1−O active center (L−Pd1−O, L=CO) generated by H2O2 oxidation. The correspondingly improved electron density over Pd−O pair renders a favorable heterolytic dissociation of C−H bond with low energy barrier of 0.48 eV. Applying CO decoration strategy to M1‐ZSM‐5 (M=Pd, Rh, Ru, Fe) enables improvement of oxygenates productivity by 3.2–11.3 times, highlighting the generalizability of this method in tuning metal‐oxo electronic structure of SACs for efficient DMC process. [ABSTRACT FROM AUTHOR]
- Subjects :
- *ACTIVATION energy
*ELECTRON density
*CATALYSTS
*METHANE
*ELECTRONIC structure
Subjects
Details
- Language :
- English
- ISSN :
- 14337851
- Volume :
- 63
- Issue :
- 16
- Database :
- Academic Search Index
- Journal :
- Angewandte Chemie International Edition
- Publication Type :
- Academic Journal
- Accession number :
- 176535569
- Full Text :
- https://doi.org/10.1002/anie.202315343