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Title: Mechanochemical reactions and hydrogen storage capacities in MBH 4–SiS 2 systems (M=Li or Na)

Abstract

The hydrogen storage properties, and phase compositions of mechanochemically prepared mixtures of xMBH 4-SiS 2 (x = 2–8), where M = Li or Na, were investigated using gas sorption analysis, powder X-ray diffraction, and infrared and solid-state NMR spectroscopic methods. The 2LiBH 4:1SiS 2 system forms an amorphous product that releases ca. 4.3 wt % of H 2 below 385 °C with a T onset of 88 °C without detectable diborane emission. The dehydrogenated sample reversibly absorbs 1.5 wt % of H 2 at 385 °C under 160 bar pressure. The H 2 release from materials with varying LiBH 4:SiS 2 ratios peaks at 8.2 wt % for the 6LiBH 4:1SiS 2 composition, with a reversible hydrogen storage capacity of 2.4 wt %. The H 2 desorption capacities of the Li-containing systems surpass those of Na-containing systems. Solid-state NMR studies indicate that products of mechanochemical reactions in the LiBH 4SiS 2 system consist of one-dimensional chains of edge-sharing SiS 4/2 tetrahedra in which the non-bridging S-ends are terminated with Li +, which are further coordinated to the [BH 4] anions. Here, a variety of possible polymorphs in the Li—Si—S-(BH 4) composition space have been identified using first principles andmore » thermodynamic modeling that supports the likelihood of formation of such novel complexes.« less

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [2];  [1];  [1]; ORCiD logo [1]
  1. Ames Lab. and Iowa State Univ., Ames, IA (United States)
  2. Univ. of Missouri, St. Louis, MO (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1506106
Report Number(s):
IS-J-9923
Journal ID: ISSN 0360-3199
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
International Journal of Hydrogen Energy
Additional Journal Information:
Journal Volume: 44; Journal Issue: 14; Journal ID: ISSN 0360-3199
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; Mechanochemistry; Hydrogen storage; Solid-state NMR

Citation Formats

Dolotko, Oleksandr, Gupta, Shalabh, Kobayashi, Takeshi, McDonald, Eric, Hlova, Ihor, Majzoub, Eric, Balema, Viktor P., Pruski, Marek, and Pecharsky, Vitalij K. Mechanochemical reactions and hydrogen storage capacities in MBH4–SiS2 systems (M=Li or Na). United States: N. p., 2019. Web. doi:10.1016/j.ijhydene.2019.01.211.
Dolotko, Oleksandr, Gupta, Shalabh, Kobayashi, Takeshi, McDonald, Eric, Hlova, Ihor, Majzoub, Eric, Balema, Viktor P., Pruski, Marek, & Pecharsky, Vitalij K. Mechanochemical reactions and hydrogen storage capacities in MBH4–SiS2 systems (M=Li or Na). United States. doi:10.1016/j.ijhydene.2019.01.211.
Dolotko, Oleksandr, Gupta, Shalabh, Kobayashi, Takeshi, McDonald, Eric, Hlova, Ihor, Majzoub, Eric, Balema, Viktor P., Pruski, Marek, and Pecharsky, Vitalij K. Sat . "Mechanochemical reactions and hydrogen storage capacities in MBH4–SiS2 systems (M=Li or Na)". United States. doi:10.1016/j.ijhydene.2019.01.211.
@article{osti_1506106,
title = {Mechanochemical reactions and hydrogen storage capacities in MBH4–SiS2 systems (M=Li or Na)},
author = {Dolotko, Oleksandr and Gupta, Shalabh and Kobayashi, Takeshi and McDonald, Eric and Hlova, Ihor and Majzoub, Eric and Balema, Viktor P. and Pruski, Marek and Pecharsky, Vitalij K.},
abstractNote = {The hydrogen storage properties, and phase compositions of mechanochemically prepared mixtures of xMBH4-SiS2 (x = 2–8), where M = Li or Na, were investigated using gas sorption analysis, powder X-ray diffraction, and infrared and solid-state NMR spectroscopic methods. The 2LiBH4:1SiS2 system forms an amorphous product that releases ca. 4.3 wt % of H2 below 385 °C with a Tonset of 88 °C without detectable diborane emission. The dehydrogenated sample reversibly absorbs 1.5 wt % of H2 at 385 °C under 160 bar pressure. The H2 release from materials with varying LiBH4:SiS2 ratios peaks at 8.2 wt % for the 6LiBH4:1SiS2 composition, with a reversible hydrogen storage capacity of 2.4 wt %. The H2 desorption capacities of the Li-containing systems surpass those of Na-containing systems. Solid-state NMR studies indicate that products of mechanochemical reactions in the LiBH4SiS2 system consist of one-dimensional chains of edge-sharing SiS4/2 tetrahedra in which the non-bridging S-ends are terminated with Li+, which are further coordinated to the [BH4]– anions. Here, a variety of possible polymorphs in the Li—Si—S-(BH4) composition space have been identified using first principles and thermodynamic modeling that supports the likelihood of formation of such novel complexes.},
doi = {10.1016/j.ijhydene.2019.01.211},
journal = {International Journal of Hydrogen Energy},
number = 14,
volume = 44,
place = {United States},
year = {2019},
month = {2}
}

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This content will become publicly available on February 16, 2020
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