| Autor: |
Gerald Charles Tustin, Yong Wang, Lawrence F. Allard, Joseph Robert Zoeller, Robert A. Dagle, Ja Hun Kwak |
| Rok vydání: |
2015 |
| Předmět: |
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| Zdroj: |
The journal of physical chemistry letters. 5(3) |
| ISSN: |
1948-7185 |
| Popis: |
We report that when Ir and La halides are deposited on carbon, exposure to CO spontaneously generates a discrete molecular heterobimetallic structure, containing an Ir-La covalent bond that acts as a highly active, selective, and stable heterogeneous catalyst for the carbonylation of methanol to produce acetic acid. This catalyst exhibits a very high productivity of ∼1.5 mol acetyl/mol Ir·s with >99% selectivity to acetyl (acetic acid and methyl acetate) without detectable loss in activity or selectivity for more than 1 month of continuous operation. The enhanced activity can be mechanistically rationalized by the presence of La within the ligand sphere of the discrete molecular Ir-La heterobimetallic structure, which acts as a Lewis acid to accelerate the normally rate-limiting CO insertion in Ir-catalyzed carbonylation. Similar approaches may provide opportunities for attaining molecular (single site) behavior similar to homogeneous catalysis on heterogeneous surfaces for other industrial applications. |
| Databáze: |
OpenAIRE |
| Externí odkaz: |
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