Crystal Structure Prediction and Dehydrogenation Mechanism of LiMg(BH4)3(NH3)2

Gözde İniş Demir; Riccarda Caputo; Samet Demir; Adem Tekin

doi:10.1021/acs.jpcc.1c00127

Crystal Structure Prediction and Dehydrogenation Mechanism of LiMg(BH₄)₃(NH₃)₂

Gözde İniş Demir, Riccarda Caputo, Samet Demir, Adem Tekin^*

^*Corresponding author for this work

Informatics Institute

Research output: Contribution to journal › Article › peer-review

4 Citations (Scopus)

Abstract

Dual-cation ammine metal borohydrides are favorable hydrogen storage materials due to their high gravimetric density and relatively low hydrogen release temperature. By combining the Fast and Flexible CrystAl Structure Predictor with density functional theory calculations and Car-Parrinello molecular dynamics, we studied the polymorphism, the lattice stability, and the decomposition mechanism of LiMg(BH4)3(NH3)2 in the temperature range 100-700 K. The onset of H2(g) formation is found at 400 K through the recombination of the hydrogen atoms from the bond cleavage of B-H and N-H in BH4 and NH3 groups. In addition to two hexagonal structures, of which one is the global minimum structure (P63/m)) and the other corresponds to the experimentally proposed room-temperature structure (P63), a monoclinic (Cc) structure and two orthorhombic structures (Fmm2, Ima2) are proposed as stable structures.

Original language	English
Pages (from-to)	10235-10242
Number of pages	8
Journal	Journal of Physical Chemistry C
Volume	125
Issue number	19
DOIs	https://doi.org/10.1021/acs.jpcc.1c00127
Publication status	Published - 20 May 2021

Bibliographical note

Publisher Copyright:
© 2021 American Chemical Society.

Funding

This work was financially supported by the Scientific and Technological Research Council of Turkey (TÜBİTAK-112T988). Computing resources in this work are provided by the National Center for High Performance Computing of Turkey (UHEM), under the Grant Number 1002132012 and Informatics Institute of İstanbul Technical University.

Funders	Funder number
Informatics Institute of İstanbul Technical University
Türkiye Bilimsel ve Teknolojik Araştirma Kurumu	1002132012, TÜBİTAK-112T988

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10.1021/acs.jpcc.1c00127

Cite this

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abstract = "Dual-cation ammine metal borohydrides are favorable hydrogen storage materials due to their high gravimetric density and relatively low hydrogen release temperature. By combining the Fast and Flexible CrystAl Structure Predictor with density functional theory calculations and Car-Parrinello molecular dynamics, we studied the polymorphism, the lattice stability, and the decomposition mechanism of LiMg(BH4)3(NH3)2 in the temperature range 100-700 K. The onset of H2(g) formation is found at 400 K through the recombination of the hydrogen atoms from the bond cleavage of B-H and N-H in BH4 and NH3 groups. In addition to two hexagonal structures, of which one is the global minimum structure (P63/m)) and the other corresponds to the experimentally proposed room-temperature structure (P63), a monoclinic (Cc) structure and two orthorhombic structures (Fmm2, Ima2) are proposed as stable structures.",

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AU - İniş Demir, Gözde

AU - Caputo, Riccarda

AU - Demir, Samet

AU - Tekin, Adem

PY - 2021/5/20

Y1 - 2021/5/20

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AB - Dual-cation ammine metal borohydrides are favorable hydrogen storage materials due to their high gravimetric density and relatively low hydrogen release temperature. By combining the Fast and Flexible CrystAl Structure Predictor with density functional theory calculations and Car-Parrinello molecular dynamics, we studied the polymorphism, the lattice stability, and the decomposition mechanism of LiMg(BH4)3(NH3)2 in the temperature range 100-700 K. The onset of H2(g) formation is found at 400 K through the recombination of the hydrogen atoms from the bond cleavage of B-H and N-H in BH4 and NH3 groups. In addition to two hexagonal structures, of which one is the global minimum structure (P63/m)) and the other corresponds to the experimentally proposed room-temperature structure (P63), a monoclinic (Cc) structure and two orthorhombic structures (Fmm2, Ima2) are proposed as stable structures.

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