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First-Principles Analysis of Elementary Steps in the Catalytic Decomposition of NO by Cu-Exchanged Zeolites
 

Summary: LETTERS
First-Principles Analysis of Elementary Steps in the Catalytic Decomposition of NO by
Cu-Exchanged Zeolites
W. F. Schneider* and K. C. Hass
Ford Research Laboratory, MD 3083/SRL, Dearborn, Michigan 48121-2053
R. Ramprasad
Department of Materials Science and Engineering, UniVersity of Illinois, Urbana, Illinois 61801
J. B. Adams
Department of Chemical, Bio and Materials Engineering, Arizona State UniVersity, Tempe, Arizona 85287
ReceiVed: January 14, 1997; In Final Form: April 10, 1997X
First-principles quantum calculations are potentially of great value for assessing the plausibility of proposed
catalytic reaction mechanisms. The present analysis of reaction pathways and energetics for key elementary
steps in the catalytic decomposition of NO to N2 + O2 by Cu-exchanged zeolites yields novel insights into
this widely studied reaction. We find evidence for a pathway involving two successive O-atom transfers to
an isolated, zeolite-bound Cu+ center, initiated by formation of a short-lived and difficult to detect isonitrosyl
intermediate, and yielding sequentially N2O and Cu-bound O followed by N2 and Cu-bound O2. The
calculations allow us to identify a complete catalytic cycle with reasonable energetics.
Introduction
Catalytic reactions often proceed by a complex series of
elementary steps that are difficult to discern experimentally. The

  

Source: Adams, James B - Department of Chemical and Materials Engineering, Arizona State University

 

Collections: Materials Science