Insight into the direct conversion of methane to methanol on modified ZIF-204 from the perspective of DFT-based calculations.

ABSTRACT: Direct oxidation of methane over oxo-doped ZIF-204, a bio-mimetic metal-organic framework, is investigated under first-principles calculations based on density functional theory. In the pristine ZIF-204, the tetrahedral methane molecule anchors to an open monocopper site via the so-called η² configuration with a physisorption energy of 0.24 eV. This weak binding arises from an electrostatic interaction between the negative charge of carbon in the methane molecule and the positive Cu²⁺ cation in the framework. In the modified ZIF-204, the doped oxo species is stabilized at the axial position of a CuN₄-base square pyramid at a distance of 2.06 Å. The dative covalent bond between Cu and oxo is responsible for the formation energy of 1.06 eV. With the pr

SUBMITTER: Le TN 

PROVIDER: S-EPMC10214002 | biostudies-literature | 2023 May

REPOSITORIES: biostudies-literature