A DFT Study of CO Hydrogenation on Graphene Oxide: Effects of Adding Mn on Fischer–Tropsch Synthesis

Author:

Bakhtiari Hanieh1,Sarabadani Tafreshi Saeedeh12ORCID,Torkashvand Mostafa1ORCID,Abdouss Majid1ORCID,de Leeuw Nora H.23ORCID

Affiliation:

1. Department of Chemistry, Amirkabir University of Technology, No. 350, Hafez Avenue, Valiasr Square, Tehran 1591634311, Iran

2. School of Chemistry, University of Leeds, Leeds LS2 9JT, UK

3. Department of Earth Sciences, Utrecht University, 3584 CB Utrecht, The Netherlands

Abstract

The hydrogenation of carbon monoxide (CO) offers a promising avenue for reducing air pollution and promoting a cleaner environment. Moreover, by using suitable catalysts, CO can be transformed into valuable hydrocarbons. In this study, we elucidate the mechanistic aspects of the catalytic conversion of CO to hydrocarbons on the surface of manganese-doped graphene oxide (Mn-doped GO), where the GO surface includes one OH group next to one Mn adatom. To gain insight into this process, we have employed calculations based on the density functional theory (DFT) to explore both the thermodynamic properties and reaction energy barriers. The Mn adatoms were found to significantly activate the catalyst surface by providing stronger adsorption geometries. Our study concentrated on two mechanisms for CO hydrogenation, resulting in either CH4 production via the reaction sequence CO → HCO → CH2O → CH2OH → CH2 → CH3 → CH4 or CH3OH formation through the CO → HCO → CH2O → CH2OH → CH3OH pathway. The results reveal that both products are likely to be formed on the Mn-doped GO surface on both thermodynamic grounds and considering the reaction energy barriers. Furthermore, the activation energies associated with each stage of the synthesis show that the conversion reactions of CH2 + OH → CH3 + O and CH2O + OH → CH2OH + O with energy barriers of 0.36 and 3.86 eV are the fastest and slowest reactions, respectively. The results also indicate that the reactions: CH2OH + OH → CH2 + O + H2O and CH2OH + OH → CH3OH + O are the most exothermic and endothermic reactions with reaction energies of −0.18 and 1.21 eV, respectively, in the catalytic pathways.

Funder

Iran National Science Foundation

UK Royal Society for an International Exchanges grant

Publisher

MDPI AG

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