• Šmíd, Břetislav
• Duchoň, Tomáš
• Weckhuysen, Bm Bert
• Jenkinson, Kellie
• Louwen, Jaap N.
• Melcherts, Angela E. M.
• Monai, Matteo
• Aert, Sandra Van
• Berben, Peter
• Groeneveld, Esther
• Altantzis, Thomas
• Bals, Sara
• Vogt, Charlotte
• Irmak, Ece A.
• Stam, Ward Van Der

Abstract

<p>Reducible supports can affect the performance of metal catalysts by the formation of suboxide overlayers upon reduction, a process referred to as the strong metal-support interaction (SMSI). A combination of operando electron microscopy and vibrational spectroscopy revealed that thin TiOx overlayers formed on nickel/titanium dioxide catalysts during 400°C reduction were completely removed under carbon dioxide hydrogenation conditions. Conversely, after 600°C reduction, exposure to carbon dioxide hydrogenation reaction conditions led to only partial reexposure of nickel, forming interfacial sites in contact with TiOx and favoring carbon-carbon coupling by providing a carbon species reservoir. Our findings challenge the conventional understanding of SMSIs and call for more-detailed operando investigations of nanocatalysts at the single-particle level to revisit static models of structure-activity relationships.</p>

Topics

• nanoparticle
• Carbon
• nickel
• titanium
• forming
• electron microscopy
• interfacial
• vibrational spectroscopy