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Title: A Discovery of Strong Metal–Support Bonding in Nanoengineered Au–Fe 3 O 4 Dumbbell-like Nanoparticles by in Situ Transmission Electron Microscopy

Abstract

The strength of metal-support bonding in heterogeneous catalysts determines their thermal stability, therefore, a tremendous amount of effort has been expended to understand metal-support interactions. Herein, we report the discovery of an anomalous “strong metal-support bonding” between gold nanoparticles and “nano-engineered” Fe 3O 4 substrates by in-situ microscopy. During in-situ vacuum annealing of Au-Fe 3O 4 dumbbell-like nanoparticles, synthesized by the epitaxial growth of nano-Fe 3O 4 on Au nanoparticles, the gold nanoparticles transform into the monolayered gold thinfilms and wet the surface of nano-Fe 3O 4, as the surface reduction of nano-Fe 3O 4 proceeds. This phenomenon results from a unique coupling of the size-and shape-dependent high surface reducibility of nano-Fe 3O 4 and the extremely strong adhesion between Au and the reduced Fe 3O 4. This strong-metal support bonding reveals the significance of controlling the metal oxide support size and morphology for optimizing metal-support bonding and, ultimately, for the development of improved catalysts and functional nanostructures.

Authors:
 [1];  [1];  [1];  [1];  [2];  [1];  [3];  [3];  [1];  [2];  [1];  [1];  [1]
  1. Purdue Univ., West Lafayette, IN (United States)
  2. Johns Hopkins Univ., Baltimore, MD (United States). Dept. of Chemical and Biomolecular Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1399979
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 17; Journal Issue: 8; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Han, Chang Wan, Choksi, Tej, Milligan, Cory, Majumdar, Paulami, Manto, Michael, Cui, Yanran, Sang, Xiahan, Unocic, Raymond R., Zemlyanov, Dmitry, Wang, Chao, Ribeiro, Fabio H., Greeley, Jeffrey, and Ortalan, Volkan. A Discovery of Strong Metal–Support Bonding in Nanoengineered Au–Fe 3 O 4 Dumbbell-like Nanoparticles by in Situ Transmission Electron Microscopy. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b00827.
Han, Chang Wan, Choksi, Tej, Milligan, Cory, Majumdar, Paulami, Manto, Michael, Cui, Yanran, Sang, Xiahan, Unocic, Raymond R., Zemlyanov, Dmitry, Wang, Chao, Ribeiro, Fabio H., Greeley, Jeffrey, & Ortalan, Volkan. A Discovery of Strong Metal–Support Bonding in Nanoengineered Au–Fe 3 O 4 Dumbbell-like Nanoparticles by in Situ Transmission Electron Microscopy. United States. doi:10.1021/acs.nanolett.7b00827.
Han, Chang Wan, Choksi, Tej, Milligan, Cory, Majumdar, Paulami, Manto, Michael, Cui, Yanran, Sang, Xiahan, Unocic, Raymond R., Zemlyanov, Dmitry, Wang, Chao, Ribeiro, Fabio H., Greeley, Jeffrey, and Ortalan, Volkan. Mon . "A Discovery of Strong Metal–Support Bonding in Nanoengineered Au–Fe 3 O 4 Dumbbell-like Nanoparticles by in Situ Transmission Electron Microscopy". United States. doi:10.1021/acs.nanolett.7b00827. https://www.osti.gov/servlets/purl/1399979.
@article{osti_1399979,
title = {A Discovery of Strong Metal–Support Bonding in Nanoengineered Au–Fe 3 O 4 Dumbbell-like Nanoparticles by in Situ Transmission Electron Microscopy},
author = {Han, Chang Wan and Choksi, Tej and Milligan, Cory and Majumdar, Paulami and Manto, Michael and Cui, Yanran and Sang, Xiahan and Unocic, Raymond R. and Zemlyanov, Dmitry and Wang, Chao and Ribeiro, Fabio H. and Greeley, Jeffrey and Ortalan, Volkan},
abstractNote = {The strength of metal-support bonding in heterogeneous catalysts determines their thermal stability, therefore, a tremendous amount of effort has been expended to understand metal-support interactions. Herein, we report the discovery of an anomalous “strong metal-support bonding” between gold nanoparticles and “nano-engineered” Fe3O4 substrates by in-situ microscopy. During in-situ vacuum annealing of Au-Fe3O4 dumbbell-like nanoparticles, synthesized by the epitaxial growth of nano-Fe3O4 on Au nanoparticles, the gold nanoparticles transform into the monolayered gold thinfilms and wet the surface of nano-Fe3O4, as the surface reduction of nano-Fe3O4 proceeds. This phenomenon results from a unique coupling of the size-and shape-dependent high surface reducibility of nano-Fe3O4 and the extremely strong adhesion between Au and the reduced Fe3O4. This strong-metal support bonding reveals the significance of controlling the metal oxide support size and morphology for optimizing metal-support bonding and, ultimately, for the development of improved catalysts and functional nanostructures.},
doi = {10.1021/acs.nanolett.7b00827},
journal = {Nano Letters},
number = 8,
volume = 17,
place = {United States},
year = {Mon Jun 26 00:00:00 EDT 2017},
month = {Mon Jun 26 00:00:00 EDT 2017}
}

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