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Critical Role of Al Pair Sites in Methane Oxidation to Methanol on Cu-Exchanged Mordenite Zeolites
| Content Provider | MDPI |
|---|---|
| Author | Han, Peijie Zhang, Zhaoxia Chen, Zheng Lin, Jingdong Wan, Shaolong Wang, Yong Wang, Shuai |
| Copyright Year | 2021 |
| Description | Cu-exchanged aluminosilicate zeolites have been intensively studied for the selective oxidation of methane to methanol via a chemical looping manner, while the nature of active Cu-oxo species for these catalysts is still under debate. This study inquired into the effects of Al distribution on methane oxidation over Cu-exchanged aluminosilicate zeolites, which provided an effective way to discern the activity difference between mononuclear and polynuclear Cu-oxo species. Specifically, conventional $Na^{+}/Co^{2+}$ ion-exchange methods were applied to quantify isolated Al and Al pair (i.e., $Al−OH−(Si−O)_{1}$–3−Al−OH) sites for three mordenite (MOR) zeolites, and a correlation was established between the reactivity of the resultant Cu-MOR catalysts and the portions of the accessible framework Al sites. These results indicated that the Cu-oxo clusters derived from the Al pair sites were more reactive than the CuOH species grafted at the isolated Al sites, which is consistent with in situ ultraviolet-visible spectroscopic characterization and density functional theory calculations. Further theoretical analysis of the first C–H bond cleavage in methane on these Cu-oxo species unveiled that stabilization of the formed methyl group was the predominant factor in determining the reactivity of methane oxidation. |
| Starting Page | 751 |
| e-ISSN | 20734344 |
| DOI | 10.3390/catal11060751 |
| Journal | Catalysts |
| Issue Number | 6 |
| Volume Number | 11 |
| Language | English |
| Publisher | MDPI |
| Publisher Date | 2021-06-19 |
| Access Restriction | Open |
| Subject Keyword | Catalysts Atomic, Molecular and Chemical Physics Methane Oxidation Methanol Mordenite Zeolite Cu-oxo Species Al Pair Site C–h Activation |
| Content Type | Text |
| Resource Type | Article |
