Towards direct synthesis of alane: A predicted defect-mediated pathway confirmed experimentally

Wang, Lin -Lin; Herwadkar, Aditi; Reich, Jason M.; Johnson, Duane D.; House, Stephen D.; Pena-Martin, Pamela; Rockett, Angus A.; Robertson, Ian M.; Gupta, Shalabh; Pecharsky, Vitalij K.

doi:10.1002/cssc.201600338

Title: Towards direct synthesis of alane: A predicted defect-mediated pathway confirmed experimentally

Journal Article · Thu Aug 18 00:00:00 EDT 2016 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.201600338· OSTI ID:1321966

^[1]; Herwadkar, Aditi ^[1]; Reich, Jason M. ^[2];

^[3];

^[4]; Pena-Martin, Pamela ^[5]; Rockett, Angus A. ^[5];

^[6]; Gupta, Shalabh ^[1];

^[7]

Ames Lab., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Univ. of Illinois Urbana-Champaign, Urbana, IL (United States)
Univ. of Illinois Urbana-Champaign, Urbana, IL (United States); Ames Lab. and Iowa State Univ., Ames, IA (United States)
Univ. of Illinois Urbana-Champaign, Urbana, IL (United States); Univ. of Pittsburgh, Pittsburgh, PA (United States)
Univ. of Illinois Urbana-Champaign, Urbana, IL (United States)
Univ. of Illinois Urbana-Champaign, Urbana, IL (United States); Univ. of Wisconsin, Madison, WI (United States)
Ames Lab. and Iowa State Univ., Ames, IA (United States)

Abstract Alane (AlH ₃ ) 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 H ₂ and (2) alane formation, which are both endothermic on a clean surface. Only with Ti dopant to facilitate H ₂ dissociation and vacancies to provide Al adatoms, both processes become exothermic. In agreement, in situ scanning tunneling microscopy showed that during H ₂ 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 AlH ₃ or closely related species at 344 bar H ₂ , indicating that the predicted pathway may lead to the direct synthesis of alane from elements at pressures much lower than the 10 ⁴ bar expected from bulk thermodynamics.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1321966

Alternate ID(s):: OSTI ID: 1786411

Report Number(s):: IS-J-025

Journal Information:: ChemSusChem, Vol. 9, Issue 17; ISSN 1864-5631

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 5 works

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