Journal
ADVANCED MATERIALS
Volume 33, Issue 44, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202104533
Keywords
atomic layer deposition; colloidal nanocrystals; heterogeneous catalysis; metal-support interactions; monolayer control
Categories
Funding
- U.S. Department of Energy, Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences [DE-AC02-76SF00515]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
- National Science Foundation [ECCS-1542152, EAR-1521055]
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The study demonstrates the importance of electronic and geometric interactions between active and support phases in heterogeneous catalysts, focusing on the challenging study of metal-support interactions. By utilizing ALD and colloidal nanocrystal synthesis methods, catalysts with sub-nanometer precision of active and support phases were prepared, allowing for detailed examination of metal-support interactions. The research highlights the significant impact of coverage and structure of Al2O3 at the Pd/Al2O3 interface on catalytic activity, with even a single monolayer of alumina contributing to a tenfold increase in reaction rate.
Electronic and geometric interactions between active and support phases are critical in determining the activity of heterogeneous catalysts, but metal-support interactions are challenging to study. Here, it is demonstrated how the combination of the monolayer-controlled formation using atomic layer deposition (ALD) and colloidal nanocrystal synthesis methods leads to catalysts with sub-nanometer precision of active and support phases, thus allowing for the study of the metal-support interactions in detail. The use of this approach in developing a fundamental understanding of support effects in Pd-catalyzed methane combustion is demonstrated. Uniform Pd nanocrystals are deposited onto Al2O3/SiO2 spherical supports prepared with control over morphology and Al2O3 layer thicknesses ranging from sub-monolayer to a approximate to 4 nm thick uniform coating. Dramatic changes in catalytic activity depending on the coverage and structure of Al2O3 situated at the Pd/Al2O3 interface are observed, with even a single monolayer of alumina contributing an order of magnitude increase in reaction rate. By building the Pd/Al2O3 interface up layer-by-layer and using uniform Pd nanocrystals, this work demonstrates the importance of controlled and tunable materials in determining metal-support interactions and catalyst activity.
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