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Reverse Spillover Dominating CO Adsorption on Single Cobalt Atoms in Graphene Divacancies
Francesco Armillotta1, Pardis Naderasli1, Valeria Chesnyak2,3
1Ecole Polytechnique Fédérale de Lausanne (EPFL), Station 3, CH-1015 Lausanne, Switzerland.
CO adsorption on single cobalt atoms in graphene primarily occurs via reverse spillover, significantly boosting sticking probability. This mechanism is crucial for understanding catalysis and gas sensing applications.
Area of Science:
- Surface Science
- Catalysis
- Materials Science
Background:
- Adsorption and desorption kinetics reveal adsorption potential and sticking probability.
- This is vital for catalysis and gas sensing applications.
- Single-atom catalysts offer unique properties for chemical reactions.
Purpose of the Study:
- Investigate room-temperature CO adsorption on single Co atoms in graphene.
- Elucidate the dominant adsorption mechanism and its impact on sticking probability.
- Determine key energy barriers involved in the adsorption process.
Main Methods:
- Utilized thermal desorption spectroscopy (TDS) for low surface density systems (<10-3 ML).
- Employed variable-temperature scanning tunneling microscopy (VT-STM).
- Applied kinetic modeling to extract energy parameters.
Main Results:
- CO adsorption on single Co atoms predominantly occurs via reverse spillover (up to 97%).
- Reverse spillover involves CO physisorption, diffusion on graphene, and lateral adsorption onto Co atoms.
- Sticking probability is enhanced by up to two orders of magnitude compared to direct impingement.
Conclusions:
- Reverse spillover is the primary CO adsorption pathway on Co/graphene single-atom catalysts.
- This mechanism significantly enhances catalytic efficiency and gas sensing capabilities.
- Quantified critical energy barriers for CO diffusion and adsorption on Co/graphene.
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