Halasz, Ivan

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  • Halasz, Ivan (2)

Author's Bibliography

Mechanochemical Synthesis and Thermal Dehydrogenation of Novel Calcium-Containing Bimetallic Amidoboranes

Milanović, Igor; Biliškov, Nikola; Užarević, Krunoslav; Lukin, Stipe; Etter, Martin; Halasz, Ivan

(2021)

TY  - JOUR
AU  - Milanović, Igor
AU  - Biliškov, Nikola
AU  - Užarević, Krunoslav
AU  - Lukin, Stipe
AU  - Etter, Martin
AU  - Halasz, Ivan
PY  - 2021
UR  - https://vinar.vin.bg.ac.rs/handle/123456789/9088
AB  - Metallic amidoboranes are widely investigated candidates for solid-state hydrogen storage, and much focus shifted recently toward bimetallic amidoboranes. Bimetallic amidoboranes are expected to introduce novel and enhanced physicochemical properties regarding storage and stability. However, these materials are still scarce and mostly grouped around magnesium- or aluminum-containing compounds. We present here a rapid and green mechanochemical solvent-free synthesis of two novel calcium-containing bimetallic amidoboranes, Li2Ca(NH2BH3)4 and Na2Ca(NH2BH3)4, from metal hydrides and ammonia borane. The insight into mechanochemical syntheses is provided by the in situ tandem synchrotron X-ray diffraction and thermal monitoring. The in situ data reveal how the choice of alkali metal hydride governs the course of reactions and their thermal profiles. In situ monitoring of thermal dehydrogenation of these materials is conducted by mass spectrometry and infrared spectroscopy, showing how the course of thermal decomposition varies depending on the structure of the amidoborane, resulting however in the same final products. These new hydrogen-rich bimetallic amidoboranes are structurally characterized by high-resolution powder X-ray diffraction, and they both show potential for hydrogen storage applications: high theoretical gravimetric capacities and low desorption temperatures of hydrogen without the significant presence of harmful gases. We also show how the choice of the milling reactor material can be decisive for the efficiency and overall success of the mechanochemical synthetic procedure, which may impact the design of milling syntheses for other thermally labile chemical systems. © 2021 American Chemical Society.
T2  - ACS Sustainable Chemistry & Engineering
T1  - Mechanochemical Synthesis and Thermal Dehydrogenation of Novel Calcium-Containing Bimetallic Amidoboranes
VL  - 9
IS  - 5
SP  - 2089
EP  - 2099
DO  - 10.1021/acssuschemeng.0c06839
ER  - 
@article{
author = "Milanović, Igor and Biliškov, Nikola and Užarević, Krunoslav and Lukin, Stipe and Etter, Martin and Halasz, Ivan",
year = "2021",
abstract = "Metallic amidoboranes are widely investigated candidates for solid-state hydrogen storage, and much focus shifted recently toward bimetallic amidoboranes. Bimetallic amidoboranes are expected to introduce novel and enhanced physicochemical properties regarding storage and stability. However, these materials are still scarce and mostly grouped around magnesium- or aluminum-containing compounds. We present here a rapid and green mechanochemical solvent-free synthesis of two novel calcium-containing bimetallic amidoboranes, Li2Ca(NH2BH3)4 and Na2Ca(NH2BH3)4, from metal hydrides and ammonia borane. The insight into mechanochemical syntheses is provided by the in situ tandem synchrotron X-ray diffraction and thermal monitoring. The in situ data reveal how the choice of alkali metal hydride governs the course of reactions and their thermal profiles. In situ monitoring of thermal dehydrogenation of these materials is conducted by mass spectrometry and infrared spectroscopy, showing how the course of thermal decomposition varies depending on the structure of the amidoborane, resulting however in the same final products. These new hydrogen-rich bimetallic amidoboranes are structurally characterized by high-resolution powder X-ray diffraction, and they both show potential for hydrogen storage applications: high theoretical gravimetric capacities and low desorption temperatures of hydrogen without the significant presence of harmful gases. We also show how the choice of the milling reactor material can be decisive for the efficiency and overall success of the mechanochemical synthetic procedure, which may impact the design of milling syntheses for other thermally labile chemical systems. © 2021 American Chemical Society.",
journal = "ACS Sustainable Chemistry & Engineering",
title = "Mechanochemical Synthesis and Thermal Dehydrogenation of Novel Calcium-Containing Bimetallic Amidoboranes",
volume = "9",
number = "5",
pages = "2089-2099",
doi = "10.1021/acssuschemeng.0c06839"
}
Milanović, I., Biliškov, N., Užarević, K., Lukin, S., Etter, M.,& Halasz, I.. (2021). Mechanochemical Synthesis and Thermal Dehydrogenation of Novel Calcium-Containing Bimetallic Amidoboranes. in ACS Sustainable Chemistry & Engineering, 9(5), 2089-2099.
https://doi.org/10.1021/acssuschemeng.0c06839
Milanović I, Biliškov N, Užarević K, Lukin S, Etter M, Halasz I. Mechanochemical Synthesis and Thermal Dehydrogenation of Novel Calcium-Containing Bimetallic Amidoboranes. in ACS Sustainable Chemistry & Engineering. 2021;9(5):2089-2099.
doi:10.1021/acssuschemeng.0c06839 .
Milanović, Igor, Biliškov, Nikola, Užarević, Krunoslav, Lukin, Stipe, Etter, Martin, Halasz, Ivan, "Mechanochemical Synthesis and Thermal Dehydrogenation of Novel Calcium-Containing Bimetallic Amidoboranes" in ACS Sustainable Chemistry & Engineering, 9, no. 5 (2021):2089-2099,
https://doi.org/10.1021/acssuschemeng.0c06839 . .
11

In-Situ and Real-time Monitoring of Mechanochemical Preparation of Li2Mg(NH2BH3)(4) and Na2Mg(NH2BH3)(4) and Their Thermal Dehydrogenation

Biliskov, Nikola; Borgschulte, Andreas; Uzarevic, Krunoslav; Halasz, Ivan; Lukin, Stipe; Milošević, Sanja S.; Milanović, Igor; Grbović-Novaković, Jasmina

(2017)

TY  - JOUR
AU  - Biliskov, Nikola
AU  - Borgschulte, Andreas
AU  - Uzarevic, Krunoslav
AU  - Halasz, Ivan
AU  - Lukin, Stipe
AU  - Milošević, Sanja S.
AU  - Milanović, Igor
AU  - Grbović-Novaković, Jasmina
PY  - 2017
UR  - http://vinar.vin.bg.ac.rs/handle/123456789/1870
AB  - For the first time, in situ monitoring of uninterrupted mechanochemical synthesis of two bimetallic amidoboranes, M2Mg(NH2BH3)(4) (M=Li, Na), by means of Raman spectroscopy, has been applied. This approach allowed real-time observation of key intermediate phases, and a straightforward follow-up of the reaction course. Detailed analysis of time-dependent spectra revealed a two-step mechanism through MNH2BH3 center dot NH3BH3 adducts as key intermediate phases which further reacted with MgH2, giving M2Mg(NH2BH3)(4) as final products. The intermediates partially take a competitive pathway toward the oligomeric M(BH3NH2BH2NH2BH3) phases. The crystal structure of the novel bimetallic amidoborane Li2Mg(NH2BH3)(4) was solved from high-resolution powder diffraction data and showed an analogous metal coordination to Na2Mg(NH2BH3)(4), but a significantly different crystal packing. Li2Mg(NH2BH3)(4) thermally dehydrogenates releasing highly pure H-2 in the amount of 7 wt.%, and at a lower temperature then its sodium analogue, making it significantly more viable for practical applications.
T2  - Chemistry. A European Journal
T1  - In-Situ and Real-time Monitoring of Mechanochemical Preparation of Li2Mg(NH2BH3)(4) and Na2Mg(NH2BH3)(4) and Their Thermal Dehydrogenation
VL  - 23
IS  - 64
SP  - 16274
EP  - 16282
DO  - 10.1002/chem.201702665
ER  - 
@article{
author = "Biliskov, Nikola and Borgschulte, Andreas and Uzarevic, Krunoslav and Halasz, Ivan and Lukin, Stipe and Milošević, Sanja S. and Milanović, Igor and Grbović-Novaković, Jasmina",
year = "2017",
abstract = "For the first time, in situ monitoring of uninterrupted mechanochemical synthesis of two bimetallic amidoboranes, M2Mg(NH2BH3)(4) (M=Li, Na), by means of Raman spectroscopy, has been applied. This approach allowed real-time observation of key intermediate phases, and a straightforward follow-up of the reaction course. Detailed analysis of time-dependent spectra revealed a two-step mechanism through MNH2BH3 center dot NH3BH3 adducts as key intermediate phases which further reacted with MgH2, giving M2Mg(NH2BH3)(4) as final products. The intermediates partially take a competitive pathway toward the oligomeric M(BH3NH2BH2NH2BH3) phases. The crystal structure of the novel bimetallic amidoborane Li2Mg(NH2BH3)(4) was solved from high-resolution powder diffraction data and showed an analogous metal coordination to Na2Mg(NH2BH3)(4), but a significantly different crystal packing. Li2Mg(NH2BH3)(4) thermally dehydrogenates releasing highly pure H-2 in the amount of 7 wt.%, and at a lower temperature then its sodium analogue, making it significantly more viable for practical applications.",
journal = "Chemistry. A European Journal",
title = "In-Situ and Real-time Monitoring of Mechanochemical Preparation of Li2Mg(NH2BH3)(4) and Na2Mg(NH2BH3)(4) and Their Thermal Dehydrogenation",
volume = "23",
number = "64",
pages = "16274-16282",
doi = "10.1002/chem.201702665"
}
Biliskov, N., Borgschulte, A., Uzarevic, K., Halasz, I., Lukin, S., Milošević, S. S., Milanović, I.,& Grbović-Novaković, J.. (2017). In-Situ and Real-time Monitoring of Mechanochemical Preparation of Li2Mg(NH2BH3)(4) and Na2Mg(NH2BH3)(4) and Their Thermal Dehydrogenation. in Chemistry. A European Journal, 23(64), 16274-16282.
https://doi.org/10.1002/chem.201702665
Biliskov N, Borgschulte A, Uzarevic K, Halasz I, Lukin S, Milošević SS, Milanović I, Grbović-Novaković J. In-Situ and Real-time Monitoring of Mechanochemical Preparation of Li2Mg(NH2BH3)(4) and Na2Mg(NH2BH3)(4) and Their Thermal Dehydrogenation. in Chemistry. A European Journal. 2017;23(64):16274-16282.
doi:10.1002/chem.201702665 .
Biliskov, Nikola, Borgschulte, Andreas, Uzarevic, Krunoslav, Halasz, Ivan, Lukin, Stipe, Milošević, Sanja S., Milanović, Igor, Grbović-Novaković, Jasmina, "In-Situ and Real-time Monitoring of Mechanochemical Preparation of Li2Mg(NH2BH3)(4) and Na2Mg(NH2BH3)(4) and Their Thermal Dehydrogenation" in Chemistry. A European Journal, 23, no. 64 (2017):16274-16282,
https://doi.org/10.1002/chem.201702665 . .
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