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 Nordlund; Flyura Djurabekova; Panagiotis Grammatikopoulos; Mukhles Sowwan

doi:10.1021/acs.chemmater.7b02242

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 Nordlund, Flyura Djurabekova, Panagiotis Grammatikopoulos, Mukhles Sowwan^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

26 Scopus citations

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 language	English
Pages (from-to)	6153-6160
Number of pages	8
Journal	Chemistry of Materials
Volume	29
Issue number	14
DOIs	https://doi.org/10.1021/acs.chemmater.7b02242
State	Published - 25 Jul 2017
Externally published	Yes

Access to Document

10.1021/acs.chemmater.7b02242

Cite this

@article{e41ff73de15f4b238145efdb5516a152,

title = "Thermal Oxidation of Size-Selected Pd Nanoparticles Supported on CuO Nanowires: The Role of the CuO-Pd Interface",

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.",

author = "Stephan Steinhauer and Junlei Zhao and Vidyadhar Singh and Theodore Pavloudis and Joseph Kioseoglou and Kai Nordlund and Flyura Djurabekova and Panagiotis Grammatikopoulos and Mukhles Sowwan",

note = "Publisher Copyright: {\textcopyright} 2017 American Chemical Society.",

year = "2017",

month = jul,

day = "25",

doi = "10.1021/acs.chemmater.7b02242",

language = "英语",

volume = "29",

pages = "6153--6160",

journal = "Chemistry of Materials",

issn = "0897-4756",

publisher = "American Chemical Society",

number = "14",

}

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

AU - Djurabekova, Flyura

AU - Grammatikopoulos, Panagiotis

AU - Sowwan, Mukhles

PY - 2017/7/25

Y1 - 2017/7/25

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.

UR - http://www.scopus.com/inward/record.url?scp=85026296661&partnerID=8YFLogxK

U2 - 10.1021/acs.chemmater.7b02242

DO - 10.1021/acs.chemmater.7b02242

M3 - 文章

AN - SCOPUS:85026296661

SN - 0897-4756

VL - 29

SP - 6153

EP - 6160

JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 14

ER -

Thermal Oxidation of Size-Selected Pd Nanoparticles Supported on CuO Nanowires: The Role of the CuO-Pd Interface

Abstract

Access to Document

Other files and links

Fingerprint

Cite this