Samenvatting
Detailed understanding of structure sensitivity, a central theme in heterogeneous catalysis, is important to guide the synthesis of improved catalysts. Progress is hampered by our inability to accurately enumerate specific active sites on ubiquitous metal nanoparticle catalysts. We employ herein atomistic simulations based on a force field trained with quantumchemical data to sample the shape of cobalt particles as a function of their size. Algorithms rooted in pattern recognition are used to identify surface atom arrangements relevant to CO dissociation, the key step in the Fischer- Tropsch (FT) reaction. The number of step-edge sites that can catalyze C-O bond scission with a low barrier strongly increases for larger nanoparticles in the range of 1-6 nm. Combined with microkinetics of the FT reaction, we can reproduce experimental FT activity trends. The stabilization of step-edge sites correlates with increasing stability of terrace nanoislands on larger nanoparticles.
Originele taal-2 | Engels |
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Pagina's (van-tot) | 8484-8492 |
Aantal pagina's | 9 |
Tijdschrift | ACS Catalysis |
Volume | 11 |
Nummer van het tijdschrift | 14 |
DOI's | |
Status | Gepubliceerd - 28 jun. 2021 |
Bibliografische nota
Publisher Copyright:© 2021 American Chemical Society. All rights reserved.
Financiering
This work was supported by the Netherlands Center for Multiscale Catalytic Energy Conversion and NWO Gravitation program funded by the Ministry of Education, Culture and Science of the government of the Netherlands. The Netherlands Organization for Scientific Research is acknowledged for providing access to computational resources.