| Autor: |
Chauhan, Manav, Rana, Bharti, Gupta, Poorvi, Kalita, Rahul, Thadhani, Chhaya, Manna, Kuntal |
| Předmět: |
|
| Zdroj: |
Nature Communications; 11/12/2024, Vol. 15 Issue 1, p1-11, 11p |
| Abstrakt: |
Direct oxidation of methane to valuable oxygenates like alcohols and acetic acid under mild conditions poses a significant challenge due to high C‒H bond dissociation energy, facile overoxidation to CO and CO2 and the intricacy of C−H activation/C−C coupling. In this work, we develop a multifunctional iron(III) dihydroxyl catalytic species immobilized within a metal-organic framework (MOF) for selective methane oxidation into methanol or acetic acid at different reaction conditions using O2. The active-site isolation of monomeric FeIII(OH)2 species at the MOF nodes, their confinement within the porous framework, and their electron-deficient nature facilitate chemoselective C‒H oxidation, yielding methanol or acetic acid with high productivities of 38 , 592 μ mol CH 3 OH g Fe − 1 h − 1 and 81 , 043 μ mol CH 3 CO 2 H g Fe − 1 h − 1 , respectively. Experiments and theoretical calculations suggest that methanol formation occurs via a FeIII-FeI-FeIII catalytic cycle, whereas CH3CO2H is produced via hydrocarboxylation of in-situ generated CH3OH with CO2 and H2, and direct CH4 carboxylation with CO2. The development of catalytic technology for direct oxidation of methane into value-added products is highly lucrative. Here, a metal-organic framework supported mono iron(III)-dihydroxyl catalyst selectively oxidizes methane into methanol or acetic acid using only oxygen, where acetic acid formation occurs via in-situ methane carboxylation and methanol hydrocarboxylation. [ABSTRACT FROM AUTHOR] |
| Databáze: |
Complementary Index |
| Externí odkaz: |
|
Full text from SpringerLink