Campus Units

Materials Science and Engineering, Ames Laboratory

Document Type

Article

Publication Version

Accepted Manuscript

Publication Date

9-18-2016

Journal or Book Title

ChemSusChem

Volume

9

Issue

17

First Page

2358

Last Page

2364

DOI

10.1002/cssc.201600338

Abstract

Alane (AlH3) is a unique energetic material that has not found a broad practical use for over 70 years because it is difficult to synthesize directly from its elements. Using density functional theory, we examine the defect-mediated formation of alane monomers on Al(111) in a two-step process: (1) dissociative adsorption of H2 and (2) alane formation, which are both endothermic on a clean surface. Only with Ti dopant to facilitate H2 dissociation and vacancies to provide Al adatoms, both processes become exothermic. In agreement, in situ scanning tunneling microscopy showed that during H2 exposure, alane monomers and clusters form primarily in the vicinity of Al vacancies and Ti atoms. Moreover, ball milling of the Al samples with Ti (providing necessary defects) showed a 10 % conversion of Al into AlH3 or closely related species at 344 bar H2, indicating that the predicted pathway may lead to the direct synthesis of alane from elements at pressures much lower than the 104 bar expected from bulk thermodynamics.

Comments

This is the peer reviewed version of the following article: Wang, Lin‐Lin, Aditi Herwadkar, Jason M. Reich, Duane D. Johnson, Stephen D. House, Pamela Peña‐Martin, Angus A. Rockett, Ian M. Robertson, Shalabh Gupta, and Vitalij K. Pecharsky. "Towards Direct Synthesis of Alane: A Predicted Defect‐Mediated Pathway Confirmed Experimentally." ChemSusChem 9, no. 17 (2016): 2358-2364., which has been published in final form at DOI: 10.1002/cssc.201600338. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving. Posted with permission.

Copyright Owner

Wiley-VCH Verlag GmbH &Co. KGaA, Weinheim

Language

en

File Format

application/pdf

Published Version

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