Journal
CHEMICAL SCIENCE
Volume 8, Issue 3, Pages 2283-2289Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6sc04788b
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Funding
- Netherlands Organization for Scientific Research (NWO), Veni project [722.014.009, SFB 749]
- cluster of excellence Nanosystems Initiative Munich (NIM)
- EU [303419]
- CINES [609, GENCI/CT8]
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Experiments on model surfaces commonly help in identifying the structural sensitivity of catalytic reactions. Nevertheless, their conclusions do not frequently lead to devising superior real-world catalysts. For instance, this is true for single-crystal platinum electrodes and the oxygen reduction reaction (ORR), an important reaction for sustainable energy conversion. Pt(111) is substantially enhanced by steps, reaching a maximum at short terrace lengths of 3-4 atoms. Conversely, regular platinum nanoparticles with similar undercoordinated defects are less active than Pt(111) and their activity increases alongside the terrace-to-defect ratio. We show here that a model to design ORR active sites on extended surfaces can also be used to solve this apparent contradiction and provide accurate design rules for nanoparticles. Essentially, only surfaces and nanostructures with concave defects can surpass the activity of Pt(111), whereas convex defects are inactive. Importantly, only the latter are present in regular nanoparticles, which is why we design various concave nanoparticles with high activities.
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