Thermal Oxidation of Size-Selected Pd Nanoparticles Supported on CuO Nanowires

The Role of the CuO–Pd Interface

Stephan Steinhauer, Junlei Zhao, Vidyadhar Singh, Theodore Pavloudis, Joseph Kioseoglou, Kai Henrik Nordlund, Flyura Gatifovna Djurabekova, Panagiotis Grammatikopoulos, Mukhles Sowwan

Research output: Contribution to journalArticleScientificpeer-review

Abstract

The structure of heterogeneous nanocatalysts supported on metal oxide materials and their morphological changes during oxidation/reduction processes play a crucial role in determining the resulting catalytic activity. Herein, we study the thermal oxidation mechanism of Pd nanoparticles supported on CuO nanowires by combining in situ environmental transmission electron microscopy (TEM), ex situ experiments, and ab initio density functional theory (DFT) calculations. High-resolution TEM imaging assisted by geometric phase analysis enabled the analysis of partially oxidized, fully oxidized, and distinct onion-like Pd nanoparticles with subsurface dislocations. Furthermore, preferential crystalline orientations between PdO nanoparticles and the CuO nanowire support have been found. Hence, the CuO–Pd interface is crucial for the thermal oxidation of Pd nanoparticles, as corroborated by electron energy loss spectroscopy and DFT calculations. The latter revealed a considerably lower energy barrier for penetration of oxygen into the Pd lattice at the CuO–Pd interface, promoting nanoparticle oxidation. The obtained results are compared with those of literature reports on different material systems, and potential implications for catalysis and chemoresistive sensing applications are discussed.
Original languageEnglish
JournalChemistry of Materials
Volume29
Issue number14
Pages (from-to)6153–6160
Number of pages8
ISSN0897-4756
DOIs
Publication statusPublished - 26 Jun 2017
MoE publication typeA1 Journal article-refereed

Fields of Science

  • 114 Physical sciences
  • NANO-PARTICLES

Cite this

Steinhauer, Stephan ; Zhao, Junlei ; Singh, Vidyadhar ; Pavloudis, Theodore ; Kioseoglou, Joseph ; Nordlund, Kai Henrik ; Djurabekova, Flyura Gatifovna ; Grammatikopoulos, Panagiotis ; Sowwan, Mukhles. / Thermal Oxidation of Size-Selected Pd Nanoparticles Supported on CuO Nanowires : The Role of the CuO–Pd Interface. In: Chemistry of Materials. 2017 ; Vol. 29 , No. 14. pp. 6153–6160.
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abstract = "The structure of heterogeneous nanocatalysts supported on metal oxide materials and their morphological changes during oxidation/reduction processes play a crucial role in determining the resulting catalytic activity. Herein, we study the thermal oxidation mechanism of Pd nanoparticles supported on CuO nanowires by combining in situ environmental transmission electron microscopy (TEM), ex situ experiments, and ab initio density functional theory (DFT) calculations. High-resolution TEM imaging assisted by geometric phase analysis enabled the analysis of partially oxidized, fully oxidized, and distinct onion-like Pd nanoparticles with subsurface dislocations. Furthermore, preferential crystalline orientations between PdO nanoparticles and the CuO nanowire support have been found. Hence, the CuO–Pd interface is crucial for the thermal oxidation of Pd nanoparticles, as corroborated by electron energy loss spectroscopy and DFT calculations. The latter revealed a considerably lower energy barrier for penetration of oxygen into the Pd lattice at the CuO–Pd interface, promoting nanoparticle oxidation. The obtained results are compared with those of literature reports on different material systems, and potential implications for catalysis and chemoresistive sensing applications are discussed.",
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Thermal Oxidation of Size-Selected Pd Nanoparticles Supported on CuO Nanowires : The Role of the CuO–Pd Interface. / Steinhauer, Stephan; Zhao, Junlei; Singh, Vidyadhar; Pavloudis, Theodore; Kioseoglou, Joseph; Nordlund, Kai Henrik; Djurabekova, Flyura Gatifovna; Grammatikopoulos, Panagiotis; Sowwan, Mukhles.

In: Chemistry of Materials, Vol. 29 , No. 14, 26.06.2017, p. 6153–6160.

Research output: Contribution to journalArticleScientificpeer-review

TY - JOUR

T1 - Thermal Oxidation of Size-Selected Pd Nanoparticles Supported on CuO Nanowires

T2 - The Role of the CuO–Pd Interface

AU - Steinhauer, Stephan

AU - Zhao, Junlei

AU - Singh, Vidyadhar

AU - Pavloudis, Theodore

AU - Kioseoglou, Joseph

AU - Nordlund, Kai Henrik

AU - Djurabekova, Flyura Gatifovna

AU - Grammatikopoulos, Panagiotis

AU - Sowwan, Mukhles

PY - 2017/6/26

Y1 - 2017/6/26

N2 - The structure of heterogeneous nanocatalysts supported on metal oxide materials and their morphological changes during oxidation/reduction processes play a crucial role in determining the resulting catalytic activity. Herein, we study the thermal oxidation mechanism of Pd nanoparticles supported on CuO nanowires by combining in situ environmental transmission electron microscopy (TEM), ex situ experiments, and ab initio density functional theory (DFT) calculations. High-resolution TEM imaging assisted by geometric phase analysis enabled the analysis of partially oxidized, fully oxidized, and distinct onion-like Pd nanoparticles with subsurface dislocations. Furthermore, preferential crystalline orientations between PdO nanoparticles and the CuO nanowire support have been found. Hence, the CuO–Pd interface is crucial for the thermal oxidation of Pd nanoparticles, as corroborated by electron energy loss spectroscopy and DFT calculations. The latter revealed a considerably lower energy barrier for penetration of oxygen into the Pd lattice at the CuO–Pd interface, promoting nanoparticle oxidation. The obtained results are compared with those of literature reports on different material systems, and potential implications for catalysis and chemoresistive sensing applications are discussed.

AB - The structure of heterogeneous nanocatalysts supported on metal oxide materials and their morphological changes during oxidation/reduction processes play a crucial role in determining the resulting catalytic activity. Herein, we study the thermal oxidation mechanism of Pd nanoparticles supported on CuO nanowires by combining in situ environmental transmission electron microscopy (TEM), ex situ experiments, and ab initio density functional theory (DFT) calculations. High-resolution TEM imaging assisted by geometric phase analysis enabled the analysis of partially oxidized, fully oxidized, and distinct onion-like Pd nanoparticles with subsurface dislocations. Furthermore, preferential crystalline orientations between PdO nanoparticles and the CuO nanowire support have been found. Hence, the CuO–Pd interface is crucial for the thermal oxidation of Pd nanoparticles, as corroborated by electron energy loss spectroscopy and DFT calculations. The latter revealed a considerably lower energy barrier for penetration of oxygen into the Pd lattice at the CuO–Pd interface, promoting nanoparticle oxidation. The obtained results are compared with those of literature reports on different material systems, and potential implications for catalysis and chemoresistive sensing applications are discussed.

KW - 114 Physical sciences

KW - NANO-PARTICLES

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