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Experimental characterization of unimolecular water dissociative adsorption on alpha-alumina

  • alpha-Al2O3 surfaces are common in both engineered applications and the environment. Much prior work indicates that their properties, e.g., reactivity, polarity, and charge, change dramatically on interaction with water. Perhaps the simplest question that can be asked of alpha-Al2O3/water interaction is how a single water molecule interacts with the most stable alpha-Al2O3 surface: the alpha-Al2O3(0001). Over the last 15 years, a series of theoretical studies have found that water dissociatively adsorbs on alpha-Al2O3(0001) through two channels. However, to our knowledge no experimental evidence of these dissociation pathways has appeared. By combining sample preparation via supersonic molecular beam dosing, sample characterization via coherent, surface specific vibrational spectroscopy and electronic structure theory, we report the first experimental observation of reaction products of each, theoretically predicted, dissociation channel. These results thus overcome a 15 year old experiment/theory disconnect and make possible aalpha-Al2O3 surfaces are common in both engineered applications and the environment. Much prior work indicates that their properties, e.g., reactivity, polarity, and charge, change dramatically on interaction with water. Perhaps the simplest question that can be asked of alpha-Al2O3/water interaction is how a single water molecule interacts with the most stable alpha-Al2O3 surface: the alpha-Al2O3(0001). Over the last 15 years, a series of theoretical studies have found that water dissociatively adsorbs on alpha-Al2O3(0001) through two channels. However, to our knowledge no experimental evidence of these dissociation pathways has appeared. By combining sample preparation via supersonic molecular beam dosing, sample characterization via coherent, surface specific vibrational spectroscopy and electronic structure theory, we report the first experimental observation of reaction products of each, theoretically predicted, dissociation channel. These results thus overcome a 15 year old experiment/theory disconnect and make possible a variety of intriguing experiments that promise to provide significant new insights into water/Al2O3 and water/oxide interaction more generally.show moreshow less

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Metadaten
Author:Harald Kirsch, Jonas Wirth, Yujin Tong, Martin Wolf, Peter SaalfrankORCiDGND, R. Kramer Campen
DOI:https://doi.org/10.1021/jp502106t
ISSN:1932-7447 (print)
Parent Title (English):The journal of physical chemistry : C, Nanomaterials and interfaces
Publisher:American Chemical Society
Place of publication:Washington
Document Type:Article
Language:English
Year of first Publication:2014
Year of Completion:2014
Release Date:2017/03/27
Volume:118
Issue:25
Pagenumber:8
First Page:13623
Last Page:13630
Funder:Deutsche Forschungsgemeinschaft through Collaborative Research Center Understanding of Metal Oxide/Water Systems at the Molecular Scale: Structural Evolution, Interfaces and Dissolution [1109]
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
Peer Review:Referiert