Effect of manganese on the selective catalytic hydrogenation of COx in the presence of light hydrocarbons over Ni/Al2O3: An experimental and computational study

Vahid Shadravan, Vanessa Jane Bukas, G.T. Kasun Kalhara Gunasooriya, Jason Waleson, Matthew Drewery, Joel Karibika, Jamie Jones, Eric Kennedy, Adesoji Adesina, Jens Kehlet Nørskov, Michael Stockenhuber*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

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Abstract

The promoting effect of manganese on Ni/Al2O3 catalyst for the hydrogenation of carbon oxides, in presence of light hydrocarbons, was studied. Ni/Al2O3 displayed a high activity for the complete conversion of CO and CO2 to methane and C2+ hydrocarbons. Moreover, over a discrete and relatively narrow temperature range, the net concentration of light C2+ hydrocarbons was elevated, with the exit stream containing a higher concentration of C2+ species than was present in the feed stream and the product stream being virtually free of carbon oxides. It is found that the addition of manganese can enhance the selectivity toward the production of light hydrocarbons. A series of Ni-Mn/Al2O3 catalysts, prepared with different Ni/Mn ratios, was studied. Various characterisation techniques such as XRD, CO and H2 chemisorption, in situ NO-FTIR and TPR were performed to gain insight into how the addition of Mn to the primary catalyst enhances the yield of light hydrocarbons. The origin of Mn-promotion was demonstrated through density functional theory (DFT) calculations, which revealed the favorable Mn substitution at the Ni(211) step edge sites under reducing conditions. The affinity of these Mn species toward oxidation stabilizes the CO dissociation product and thus provides a thermodynamic driving force that promotes C-O bond cleavage as compared to the Mn-unmodified catalyst surface.
Original languageEnglish
JournalA C S Catalysis
Volume10
Pages (from-to)1535-1547
ISSN2155-5435
DOIs
Publication statusPublished - 2020

Bibliographical note

This project has received Funding from the European Union's Seventh Framework Programme and Horizon 2020 Research and Innovation Programme under Marie Sklodowska-Curie Actions grant no. 713683 (H2020)

Keywords

  • CO and CO2 hydrogenation
  • Bimetallic catalysts
  • Nickel
  • Manganese
  • Density functional theory

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