In-Situ and Real-time Monitoring of Mechanochemical Preparation of Li2Mg(NH2BH3)(4) and Na2Mg(NH2BH3)(4) and Their Thermal Dehydrogenation
Само за регистроване кориснике
2017
Аутори
Biliškov, NikolaBorgschulte, Andreas
Uzarevic, Krunoslav
Halasz, Ivan
Lukin, Stipe
Milošević, Sanja S.
Milanović, Igor
Grbović-Novaković, Jasmina
Чланак у часопису (Објављена верзија)
Метаподаци
Приказ свих података о документуАпстракт
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 temperat...ure then its sodium analogue, making it significantly more viable for practical applications.
Кључне речи:
amidoboranes / hydrogen storage / mechanochemistry / Raman spectroscopy / thermal dehydrogenationИзвор:
Chemistry. A European Journal, 2017, 23, 64, 16274-16282Финансирање / пројекти:
- Синтеза, процесирање и карактеризација наноструктурних материјала за примену у области енергије, механичког инжењерства, заштите животне стредине и биомедицине (RS-MESTD-Integrated and Interdisciplinary Research (IIR or III)-45012)
- Ministry of Environment and Energy, Ministry of Science and Education, Environmental Protection and Energy Efficiency Fund, Croatian Science Foundation under the project New Materials for Energy Storage
DOI: 10.1002/chem.201702665
ISSN: 0947-6539; 1521-3765
PubMed: 28902966
WoS: 000417968100021
Scopus: 2-s2.0-85034074987
Колекције
Институција/група
VinčaTY - JOUR AU - Biliškov, 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 - https://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 = "Biliškov, 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" }
Biliškov, 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
Biliškov 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 .
Biliškov, 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 . .