Journal
NANO LETTERS
Volume 21, Issue 15, Pages 6640-6647Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c02104
Keywords
Liquid cell; in situ transmission electron microscopy; etching; surface adsorption; ligand; inhibitor molecules
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Funding
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), Materials Science and Engineering Division [DE-AC02-05-CH11231]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
- National Natural Science Foundation of China [51925903]
- National Key R&D Program of China [2018YFC0705401]
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Selective adsorption of ligands on nanocrystal surfaces affects oxidative etching. Different concentrations of iron acetylacetonate led to different etching pathways on palladium nanocrystals. Ab initio calculations showed that differences in adsorption energy of inhibitor molecules on palladium facets influenced the etching behavior.
Selective adsorption of ligands on nanocrystal surfaces can affect oxidative etching. Here, we report the etching of palladium nanocrystals imaged using liquid cell transmission electron microscopy. The adsorption of surface ligands (i.e., iron acetylacetonate and its derivatives) and their role as inhibitor molecules on the etching process were investigated. Our observations revealed that the etching was dominated by the interplay between palladium facets and ligands and that the etching exhibited different pathways at different concentrations of ligands. At a low concentration of iron acetylacetonate (0.1 mM), rapid etching primarily at {100} facets led to a concave structure. At a high concentration (1.0 mM), the etch rate was decreased owing to a protective film of iron acetylacetonate on the {100} facets and a round nanoparticle was achieved. Ab initio calculations showed that the differences in adsorption energy of inhibitor molecules on palladium facets were responsible for the etching behavior.
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