Influence of carbon support surface modification on the performance of nickel catalysts in carbon dioxide hydrogenation

• Published in: Catalysis today Vol. 418; p. 114071
• Main Authors: Visser, Nienke L., Verschoor, Juliette C., Smulders, Luc C.J., Mattarozzi, Francesco, Morgan, David J., Meeldijk, Johannes D., van der Hoeven, Jessi E.S., Stewart, Joseph A., Vandegehuchte, Bart D., de Jongh, Petra E.
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01-06-2023
• Subjects: Carbon support; CO2 hydrogenation; Functionalization; Nickel; Nickel; Functionalization; Carbon support; CO2 hydrogenation
• ISSN: 0920-5861; 1873-4308
• DOI: 10.1016/j.cattod.2023.114071

The interaction between metal nanoparticles and a support is of key importance in catalysis. In this study, we demonstrate that the introduction of oxygen- or nitrogen-containing surface groups on a graphite nanoplatelet support influences the performance of nickel supported catalysts during CO2 hydrogenation. By careful design of the synthesis conditions, the Ni nanoparticle size of the fresh catalysts was not affected by the type of support surface groups. A combination of H2 chemisorption and high resolution TEM demonstrates that the available metal surface depends on the interaction with the carbon support. The amination treatment to introduce nitrogen-containing groups results in the weakest interaction between the Ni and the support, showing the highest initial Ni weight-based activity, although at the expense of nanoparticle stability. Hence initial enhancement in activity is not always optimal for long term catalysis. The use of carbon with a higher density of oxygen functional groups that are stable above 350 °C, is beneficial for preventing deactivation due to particle growth. Furthermore, small amounts of contaminants can have a substantial influence on the CH4 selectivity at low conversions.
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•Graphite carbon platelets were functionalized with various types of support surface groups to modify their acidity/basicity.•Nickel nanoparticles with similar sizes were supported on these carbon materials.•Nickel on aminated carbon was initially the most active in high pressure CO2 hydrogenation, but the least stable.•Introduction of oxygen-containing surface groups greatly enhanced the catalyst stability.•Support functionalization improved the CH4 selectivity, although type of support surface groups present did not matter.