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Nanoscale Spatial Distribution of Supported Nanoparticles Controls Activity and Stability in Powder Catalysts for CO Oxidation and Photocatalytic H2 Evolution

Holm, Alexander (författare)
Stockholms universitet,Fysikum,Department of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, California 94305, United States;Department of Physics, AlbaNova University Center, Stockholm University, Stockholm SE-106 91, Sweden
Goodman, Emmett D. (författare)
Department of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, California 94305, United States
Halldin Stenlid, Joakim (författare)
Stockholms universitet,Fysikum,Department of Physics, AlbaNova University Center, Stockholm University, Stockholm SE-106 91, Sweden
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Aitbekova, Aisulu (författare)
Department of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, California 94305, United States
Zelaya, Rosadriana (författare)
Department of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, California 94305, United States
Diroll, Benjamin T. (författare)
Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois 60439, United States
Johnston-Peck, Aaron C. (författare)
Material Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, United States
Kao, Kun-Che (författare)
Department of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, California 94305, United States
Frank, Curtis W. (författare)
Department of Chemical Engineering, Stanford University, Stanford, California 94305, United States
Pettersson, Lars G.M. (författare)
Stockholms universitet,Fysikum,Department of Physics, AlbaNova University Center, Stockholm University, Stockholm SE-106 91, Sweden
Cargnello, Matteo (författare)
Department of Chemical Engineering and SUNCAT Center for Interface Science and Catalysis, Stanford University, Stanford, California 94305, United States
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 (creator_code:org_t)
2020-07-30
2020
Engelska.
Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 142:34, s. 14481-14494
Relaterad länk:
https://www.ncbi.nlm...
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https://urn.kb.se/re...
https://doi.org/10.1...
https://urn.kb.se/re...
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  • Tidskriftsartikel (refereegranskat)
Abstract Ämnesord
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  • Supported metal nanoparticles are essential components of high-performing catalysts, and their structures are intensely researched. In comparison, nanoparticle spatial distribution in powder catalysts is conventionally not quantified, and the influence of this collective property on catalyst performance remains poorly investigated. Here, we demonstrate a general colloidal self-assembly method to control uniformity of nanoparticle spatial distribution on common industrial powder supports. We quantify distributions on the nanoscale using image statistics and show that the type of nanospatial distribution determines not only the stability, but also the activity of heterogeneous catalysts. Widely investigated systems (Au–TiO2 for CO oxidation thermocatalysis and Pd–TiO2 for H2 evolution photocatalysis) were used to showcase the universal importance of nanoparticle spatial organization. Spatially and temporally resolved microkinetic modeling revealed that nonuniformly distributed Au nanoparticles suffer from local depletion of surface oxygen, and therefore lower CO oxidation activity, as compared to uniformly distributed nanoparticles. Nanoparticle spatial distribution also determines the stability of Pd–TiO2 photocatalysts, because nonuniformly distributed nanoparticles sinter while uniformly distributed nanoparticles do not. This work introduces new tools to evaluate and understand catalyst collective (ensemble) properties in powder catalysts, which thereby pave the way to more active and stable heterogeneous catalysts.

Ämnesord

NATURVETENSKAP  -- Kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)
NATURVETENSKAP  -- Kemi -- Annan kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Other Chemistry Topics (hsv//eng)

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