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Title: Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution

Abstract

A novel pathway of increasing the surface density of catalytically active oxygen radical sites on a MoVTeNb oxide (M1 phase) catalyst during alkane oxidative dehydrogenation is reported. The novel sites form when a fraction of Te4+ is reduced and emitted from the M1 crystals under catalytic operating conditions, without compromising structural integrity of the catalyst framework. Density functional theory calculations show this Te reduction induces multiple inter-related electron transfers, and the associated cooperative effects lead to the formation of O- radicals. The in situ observations identify complex dynamic changes in the catalyst on an atomistic level, highlighting a new way to tailor structure and dynamics for highly active catalysts.

Authors:
ORCiD logo; ;  [1]; ; ;  [2];  [1]; ORCiD logo [1];  [3]
  1. Department of Chemistry and Catalysis Research Center, Technische Universität München, Garching 85748, Germany
  2. National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  3. Department of Materials Science and Engineering, University of Washington, Seattle, Washington 98195, United States
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1398226
Report Number(s):
PNNL-SA-129307
Journal ID: ISSN 0002-7863; 48583
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 36; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Zhu, Yuanyuan, Sushko, Peter V., Melzer, Daniel, Jensen, Eric, Kovarik, Libor, Ophus, Colin, Sanchez-Sanchez, Maricruz, Lercher, Johannes A., and Browning, Nigel D. Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution. United States: N. p., 2017. Web. doi:10.1021/jacs.7b05240.
Zhu, Yuanyuan, Sushko, Peter V., Melzer, Daniel, Jensen, Eric, Kovarik, Libor, Ophus, Colin, Sanchez-Sanchez, Maricruz, Lercher, Johannes A., & Browning, Nigel D. Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution. United States. doi:10.1021/jacs.7b05240.
Zhu, Yuanyuan, Sushko, Peter V., Melzer, Daniel, Jensen, Eric, Kovarik, Libor, Ophus, Colin, Sanchez-Sanchez, Maricruz, Lercher, Johannes A., and Browning, Nigel D. Tue . "Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution". United States. doi:10.1021/jacs.7b05240.
@article{osti_1398226,
title = {Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution},
author = {Zhu, Yuanyuan and Sushko, Peter V. and Melzer, Daniel and Jensen, Eric and Kovarik, Libor and Ophus, Colin and Sanchez-Sanchez, Maricruz and Lercher, Johannes A. and Browning, Nigel D.},
abstractNote = {A novel pathway of increasing the surface density of catalytically active oxygen radical sites on a MoVTeNb oxide (M1 phase) catalyst during alkane oxidative dehydrogenation is reported. The novel sites form when a fraction of Te4+ is reduced and emitted from the M1 crystals under catalytic operating conditions, without compromising structural integrity of the catalyst framework. Density functional theory calculations show this Te reduction induces multiple inter-related electron transfers, and the associated cooperative effects lead to the formation of O- radicals. The in situ observations identify complex dynamic changes in the catalyst on an atomistic level, highlighting a new way to tailor structure and dynamics for highly active catalysts.},
doi = {10.1021/jacs.7b05240},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 36,
volume = 139,
place = {United States},
year = {2017},
month = {8}
}