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Direct Hydrogenation of Dinitrogen and Dioxygen via Eley-Rideal Reactions

Yao, Yunxi and Giapis, Konstantinos P. (2016) Direct Hydrogenation of Dinitrogen and Dioxygen via Eley-Rideal Reactions. Angewandte Chemie International Edition, 55 (38). pp. 11595-11599. ISSN 1433-7851. http://resolver.caltech.edu/CaltechAUTHORS:20160819-082415704

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Abstract

Most Eley–Rideal abstraction reactions involve an energetic gas-phase atom reacting directly with a surface adsorbate to form a molecular product. Molecular projectiles are generally less reactive, may dissociate upon collision with the surface, and thus more difficult to prove that they can participate intact in abstraction reactions. Here we provide experimental evidence for direct reactions occurring between molecular N_2^+ and O_2^+ projectiles and surface-adsorbed D atoms in two steps: first, the two atoms of the diatomic molecule undergo consecutive collisions with a metal surface atom without bond rupture; and second, the rebounding molecule abstracts a surface D atom to form N_2D and O_2D intermediates, respectively, detected as ions. The kinematics of the collisional interaction confirms product formation by an Eley–Rideal reaction mechanism and accounts for inelastic energy losses commensurate with surface re-ionization. Such energetic hydrogenation of dinitrogen may provide facile activation of its triple bond as a first step towards bond cleavage.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1002/anie.201604899DOIArticle
http://onlinelibrary.wiley.com/doi/10.1002/anie.201604899/abstractPublisherArticle
ORCID:
AuthorORCID
Giapis, Konstantinos P.0000-0002-7393-298X
Additional Information:© 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. Received: May 19, 2016; Revised: July 5, 2016; First published: 18 August 2016. Funding support from the National Science Foundation is gratefully acknowledged (award number 1202567).
Funders:
Funding AgencyGrant Number
NSFPHY-1202567
Subject Keywords:Eley–Rideal reactions; hydroperoxyl; ion scattering; nitrogen activation; surface dynamics
Record Number:CaltechAUTHORS:20160819-082415704
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20160819-082415704
Official Citation:Y. Yao, K. P. Giapis, Angew. Chem. Int. Ed. 2016, 55, 11595.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:69766
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:22 Aug 2016 23:39
Last Modified:27 Sep 2016 15:54

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