4 years ago

Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution

Formation of Oxygen Radical Sites on MoVNbTeOx by Cooperative Electron Redistribution
Libor Kovarik, Peter V. Sushko, Eric Jensen, Yuanyuan Zhu, Maricruz Sanchez-Sanchez, Colin Ophus, Daniel Melzer, Nigel D. Browning, Johannes A. Lercher
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.

Publisher URL: http://dx.doi.org/10.1021/jacs.7b05240

DOI: 10.1021/jacs.7b05240

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