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Direct Experimental Observation of in situ Dehydrogenation of an Amine-Borane System Using Gas Electron Diffraction

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Direct Experimental Observation of in situ Dehydrogenation of an Amine-Borane System Using Gas Electron Diffraction. / Ja'O, Aliyu M.; Masters, Sarah L.; Wann, Derek A.; Rankine, Conor D.; Nunes, João P.F.; Guillemin, Jean Claude.

In: Journal of Physical Chemistry A, Vol. 123, No. 32, 15.08.2019, p. 7104-7112.

Research output: Contribution to journalArticlepeer-review

Harvard

Ja'O, AM, Masters, SL, Wann, DA, Rankine, CD, Nunes, JPF & Guillemin, JC 2019, 'Direct Experimental Observation of in situ Dehydrogenation of an Amine-Borane System Using Gas Electron Diffraction', Journal of Physical Chemistry A, vol. 123, no. 32, pp. 7104-7112. https://doi.org/10.1021/acs.jpca.9b05522

APA

Ja'O, A. M., Masters, S. L., Wann, D. A., Rankine, C. D., Nunes, J. P. F., & Guillemin, J. C. (2019). Direct Experimental Observation of in situ Dehydrogenation of an Amine-Borane System Using Gas Electron Diffraction. Journal of Physical Chemistry A, 123(32), 7104-7112. https://doi.org/10.1021/acs.jpca.9b05522

Vancouver

Ja'O AM, Masters SL, Wann DA, Rankine CD, Nunes JPF, Guillemin JC. Direct Experimental Observation of in situ Dehydrogenation of an Amine-Borane System Using Gas Electron Diffraction. Journal of Physical Chemistry A. 2019 Aug 15;123(32):7104-7112. https://doi.org/10.1021/acs.jpca.9b05522

Author

Ja'O, Aliyu M. ; Masters, Sarah L. ; Wann, Derek A. ; Rankine, Conor D. ; Nunes, João P.F. ; Guillemin, Jean Claude. / Direct Experimental Observation of in situ Dehydrogenation of an Amine-Borane System Using Gas Electron Diffraction. In: Journal of Physical Chemistry A. 2019 ; Vol. 123, No. 32. pp. 7104-7112.

Bibtex - Download

@article{b1f6420cc4da48678c37709c0446bd5b,
title = "Direct Experimental Observation of in situ Dehydrogenation of an Amine-Borane System Using Gas Electron Diffraction",
abstract = "In situ dehydrogenation of azetidine-BH3, which is a candidate for hydrogen storage, was observed with the parent and dehydrogenated analogue subjected to rigorous structural and thermochemical investigations. The structural analyses utilized gas electron diffraction supported by high-level quantum calculations, while the pathway for the unimolecular hydrogen release reaction in the absence and presence of BH3 as a bifunctional catalyst was predicted at the CBS-QB3 level. The catalyzed dehydrogenation pathway has a barrier lower than the predicted B-N bond dissociation energy, hence favoring the dehydrogenation process over the dissociation of the complex. The predicted enthalpy of dehydrogenation at the CCSD(T)/CBS level indicates that mild reaction conditions would be required for hydrogen release and that the compound is closer to thermoneutral than linear amine boranes. The entropy and free energy change for the dehydrogenation process show that the reaction is exergonic, energetically feasible, and will proceed spontaneously toward hydrogen release, all of which are important factors for hydrogen storage.",
author = "Ja'O, {Aliyu M.} and Masters, {Sarah L.} and Wann, {Derek A.} and Rankine, {Conor D.} and Nunes, {Jo{\~a}o P.F.} and Guillemin, {Jean Claude}",
note = "{\textcopyright} 2019 American Chemical Society. This is an author-produced version of the published paper. Uploaded in accordance with the publisher{\textquoteright}s self-archiving policy. Further copying may not be permitted; contact the publisher for details.",
year = "2019",
month = aug,
day = "15",
doi = "10.1021/acs.jpca.9b05522",
language = "English",
volume = "123",
pages = "7104--7112",
journal = "Journal of Physical Chemistry A",
issn = "1089-5639",
number = "32",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Direct Experimental Observation of in situ Dehydrogenation of an Amine-Borane System Using Gas Electron Diffraction

AU - Ja'O, Aliyu M.

AU - Masters, Sarah L.

AU - Wann, Derek A.

AU - Rankine, Conor D.

AU - Nunes, João P.F.

AU - Guillemin, Jean Claude

N1 - © 2019 American Chemical Society. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.

PY - 2019/8/15

Y1 - 2019/8/15

N2 - In situ dehydrogenation of azetidine-BH3, which is a candidate for hydrogen storage, was observed with the parent and dehydrogenated analogue subjected to rigorous structural and thermochemical investigations. The structural analyses utilized gas electron diffraction supported by high-level quantum calculations, while the pathway for the unimolecular hydrogen release reaction in the absence and presence of BH3 as a bifunctional catalyst was predicted at the CBS-QB3 level. The catalyzed dehydrogenation pathway has a barrier lower than the predicted B-N bond dissociation energy, hence favoring the dehydrogenation process over the dissociation of the complex. The predicted enthalpy of dehydrogenation at the CCSD(T)/CBS level indicates that mild reaction conditions would be required for hydrogen release and that the compound is closer to thermoneutral than linear amine boranes. The entropy and free energy change for the dehydrogenation process show that the reaction is exergonic, energetically feasible, and will proceed spontaneously toward hydrogen release, all of which are important factors for hydrogen storage.

AB - In situ dehydrogenation of azetidine-BH3, which is a candidate for hydrogen storage, was observed with the parent and dehydrogenated analogue subjected to rigorous structural and thermochemical investigations. The structural analyses utilized gas electron diffraction supported by high-level quantum calculations, while the pathway for the unimolecular hydrogen release reaction in the absence and presence of BH3 as a bifunctional catalyst was predicted at the CBS-QB3 level. The catalyzed dehydrogenation pathway has a barrier lower than the predicted B-N bond dissociation energy, hence favoring the dehydrogenation process over the dissociation of the complex. The predicted enthalpy of dehydrogenation at the CCSD(T)/CBS level indicates that mild reaction conditions would be required for hydrogen release and that the compound is closer to thermoneutral than linear amine boranes. The entropy and free energy change for the dehydrogenation process show that the reaction is exergonic, energetically feasible, and will proceed spontaneously toward hydrogen release, all of which are important factors for hydrogen storage.

UR - http://www.scopus.com/inward/record.url?scp=85071355595&partnerID=8YFLogxK

U2 - 10.1021/acs.jpca.9b05522

DO - 10.1021/acs.jpca.9b05522

M3 - Article

C2 - 31314528

VL - 123

SP - 7104

EP - 7112

JO - Journal of Physical Chemistry A

JF - Journal of Physical Chemistry A

SN - 1089-5639

IS - 32

ER -