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

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

doi:10.1021/acs.jpcc.1c00127

Cited by 4 publications

(2 citation statements)

References 58 publications

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“…In metal borohydrides, there is an electrostatic interaction between the positively charged metal and the negatively charged borohydride, which stabilizes the crystal structure. − In the CSP of covalently bonded crystals, the FFCASP tries to maximize the number of stabilizing interactions. In trimetallic borohydrides, all metal species tend to make stronger bonding interactions with borohydrides and therefore at first, a unit cell has been constructed including freely movable BH 4 groups and individual Li, Al, and Na atoms for each LiAlM(BH 4 ) x ( x = 5, 6, and 7).…”

Section: Results and Discussionmentioning

confidence: 99%

Hydrogen Storage in Trimetallic Borohydrides: a Crystal Structure Prediction and Ab Initio Molecular Dynamics Simulations Study

Demir,

Torkashvand,

Jouybar

et al. 2023

J. Phys. Chem. C

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Trimetallic borohydrides have emerged as promising candidates for hydrogen storage due to their unique structural and chemical properties. Nevertheless, the literature on trimetallic borohydrides is limited to only a few studied examples. Thermodynamic properties of trimetallic borohydrides can be tuned by changing the composition and stoichiometry of the compound. In this regard, the hydrogen storage potential of a series of new Al-based trimetallic borohydrides, including alkali, earth alkali, and transition metals with different electronegativities, with a general formula of LiAlM(BH4)5–7 (M = Na, Mg, Sc, Y, Zn, and Mo) has been investigated using various computational tools. Due to the limited knowledge about the crystal structure of trimetallic borohydrides, first, a crystal structure prediction study has been accomplished to determine the lowest-energy crystal structures of Al-based trimetallic borohydrides using the recently developed highly parallel FFCASP tool together with subsequent electronic structure calculations. Iso-energetic crystal structures with different metal-borohydride coordinations were obtained with FFCASP especially for the higher borohydride stoichiometries, indicating a potential energy landscape with shallow minima, which make easier the phase transformations under temperature. The convex hull of the ternary LiBH4–Al(BH4)3-M(BH4) x (M = Na, Mg, Zn, and Y) system indicated that while both LiAlNa(BH4)5 and LiAlZn(BH4)6 are stable, LiAlMg(BH4)6 and LiAlY(BH4)7 are metastable. Hydrogen release dynamics in these predicted structures was studied with the help of ab initio molecular dynamics (AIMD) simulations. Among the trimetallic borohydrides, AIMD simulations indicated that LiAlZn(BH4)6 has a favorable hydrogen release temperature, starting from 392 K.

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Section: Results and Discussionmentioning

confidence: 99%

Hydrogen Storage in Trimetallic Borohydrides: a Crystal Structure Prediction and Ab Initio Molecular Dynamics Simulations Study

Demir,

Torkashvand,

Jouybar

et al. 2023

J. Phys. Chem. C

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“…Recently, FFCASP, an inhouse-developed algorithm, was successfully applied to both molecular and covalent bonded crystals. [31][32][33][34] It employs a hybrid global optimization strategy including consecutive particle swarm optimization (PSO) 35 and simulated annealing (SA) 36 algorithms. FFCASP is massively parallelized with the Message Passing Interface (MPI) library by using a task-farming approach.…”

Section: Computational Detailsmentioning

confidence: 99%

Stable and metastable crystal structures and ammonia dynamics in strontium chloride ammines

Demir,

Çankaya

et al. 2023

Phys. Chem. Chem. Phys.

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2D‐FFCASP—A New Approach for 2D Structure Prediction Applied to Self‐Assemblies of DNA Bases

Demir

Tekin

2022

Advcd Theory and Sims

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Biomolecular self-assembly on surfaces is an emerging and exciting field for the fabrication of 2D nanostructures that are being used in a wide range of applications. Self-assembly of the nucleic acid bases, which are mostly stabilized by hydrogen bonding, in both solution and solid have been well characterized by various experimental techniques such as nuclear magnetic resonance (NMR) and scanning tunneling microscopy (STM). Especially for the surface based self assemblies, the resolution of STM images is quite insufficient to reveal the dominating intermolecular interactions which lead to the formation of self-assembled DNA bases. Moreover, it is also possible to form crystalline order self assemblies by finding suitable experimental conditions. This fact allows the application of crystal structure prediction (CSP) tools for the discovery of ordered self assemblies. In this regard, the existing CSP method called FFCASP has been extended with a new implementation allowing the prediction of 1D or 2D periodic and nonperiodic structures. The new approach, 2D-FFCASP, has been applied to four DNA bases and the best resulting structures have been further evaluated by dispersion-corrected density functional theory (DFT-D) and cluster in a molecule local correlation approach at the second-order Møller-Plesset perturbation (CIM-RI-MP2). 2D-FFCASP successfully reproduced the known self-assemblies of DNA bases in addition to many newly found isoenergetic structures.

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

Cited by 4 publications

References 58 publications

Hydrogen Storage in Trimetallic Borohydrides: a Crystal Structure Prediction and Ab Initio Molecular Dynamics Simulations Study

Hydrogen Storage in Trimetallic Borohydrides: a Crystal Structure Prediction and Ab Initio Molecular Dynamics Simulations Study

Stable and metastable crystal structures and ammonia dynamics in strontium chloride ammines

2D‐FFCASP—A New Approach for 2D Structure Prediction Applied to Self‐Assemblies of DNA Bases

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