Issue 16, 2022

A theoretical study on the mechanism of conversion of C3H8 and CO2 to C3H6 and HCOOH by M4–B24N28 catalysis

Abstract

The mechanism of the conversion of propane and carbon dioxide to propylene and formic acid on the M4–B24N28 (M = V, Cr, Ni, Cu) surface was studied based on density functional theory (DFT). Through the preliminary calculation of propane oxidation, it was found that Cu4–B24N28 has relatively good catalytic activity. After that, all possible paths for the oxidation reaction of propane and carbon dioxide on the surface of Cu4–B24N28 were calculated in detail. The calculation results showed that the optimal path is the dehydrogenation of the secondary carbon of propane combined with the carbon atoms of carbon dioxide to form a HCO2 intermediate, and then the secondary carbon continues to dehydrogenate to combine with the HCO2 intermediate to form a C3H6 intermediate and formic acid. After that the hydrogen atom of the primary carbon of the C3H6 intermediate is rearranged to the secondary carbon to produce propylene (CH3CH2CH3 + CO2 → CH3CHCH3 + OCHO → CH3CCH3 + HCOOH → CH2CHCH3 + HCOOH), the rate control step of the reaction process is the rearrangement of the hydrogen atom of the C3H6 intermediate, and then formic acid and propylene are desorbed with desorption energies of −0.23 eV and −0.50 eV respectively, and can be further recycled. In summary, Cu4–B24N28 can be used as an effective catalyst for the oxidation of propane by carbon dioxide, which can maintain the catalytic activity and take into account the catalytic stability without generating carbon deposits.

Graphical abstract: A theoretical study on the mechanism of conversion of C3H8 and CO2 to C3H6 and HCOOH by M4–B24N28 catalysis

Supplementary files

Article information

Article type
Paper
Submitted
30 Jan 2022
Accepted
17 Mar 2022
First published
18 Mar 2022

New J. Chem., 2022,46, 7598-7607

A theoretical study on the mechanism of conversion of C3H8 and CO2 to C3H6 and HCOOH by M4–B24N28 catalysis

J. Lv, R. Ren and Y. Lv, New J. Chem., 2022, 46, 7598 DOI: 10.1039/D2NJ00522K

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