Mechanochemical modification of LiAlH4 with Fe2O3 - A combined DFT and experimental study
Аутори
Dragojlović, MilijanaMilanović, Igor
Gradišek, Anton
Kurko, Sandra V.
Mitrić, Miodrag
Umićević, Ana
Radaković, Jana
Batalović, Katarina
Чланак у часопису (Рецензирана верзија)
Метаподаци
Приказ свих података о документуАпстракт
LiAlH4 is a promising material for hydrogen storage, having the theoretical gravimetric density of 10.6 wt% H2. In order to decrease the temperature where hydrogen is released, we investigated the catalytic influence of Fe2O3 on LiAlH4 dehydrogenation, as a model case for understanding the effects transition oxide additives have in the catalysis process. Quick mechanochemical synthesis of LiAlH4 + 5 wt% Fe2O3 led to the significant decrease of the hydrogen desorption temperature, and desorption of over 7 wt%H2 in the temperature range 143–154 °C. Density functional theory (DFT)-based calculations with Tran-Blaha modified Becke-Johnson functional (TBmBJ) address the electronic structure of LiAlH4 and Li3AlH6. 57Fe Mössbauer study shows the change in the oxidational state of iron during hydrogen desorption, while the 1H NMR study reveals the presence of paramagnetic species that affect relaxation. The electron transfer from hydrides is discussed as the proposed mechanism of destabilizati...on of LiAlH4 + 5 wt% Fe2O3. © 2021 Hydrogen Energy Publications LLC
Кључне речи:
LiAlH4 / DFT / Hydrogen storage / Fe-57 Mossbauer / H-1 NMR / Fe2O3Извор:
International Journal of Hydrogen Energy, 2021, 46, 24, 13070-13081Финансирање / пројекти:
- Ministry of Education, Science and Technological Development of the Republic of Serbia
- Slovenian Research Agency [P10125]
- Serbia-Slovenia bilateral research project [BIRS/16/17051]
Напомена:
- This is accepted peer-reviewed version of the article: Dragojlović, M., Milanović, I., Gradišek, A., Kurko, S., Mitrić, M., Umićević, A., ... & Batalović, K. (2021). Mechanochemical modification of LiAlH4 with Fe2O3-A combined DFT and experimental study. International Journal of Hydrogen Energy. http://dx.doi.org/10.1016/j.ijhydene.2021.01.086
- Published version: https://vinar.vin.bg.ac.rs/handle/123456789/9087
Повезане информације:
- Друга верзија
https://vinar.vin.bg.ac.rs/handle/123456789/9087 - Друга верзија
http://dx.doi.org/10.1016/j.ijhydene.2021.01.086
DOI: 10.1016/j.ijhydene.2021.01.086
ISSN: 0360-3199
WoS: 000632350100019
Scopus: 2-s2.0-85100961364
Колекције
Институција/група
VinčaTY - JOUR AU - Dragojlović, Milijana AU - Milanović, Igor AU - Gradišek, Anton AU - Kurko, Sandra V. AU - Mitrić, Miodrag AU - Umićević, Ana AU - Radaković, Jana AU - Batalović, Katarina PY - 2021 UR - https://vinar.vin.bg.ac.rs/handle/123456789/9091 AB - LiAlH4 is a promising material for hydrogen storage, having the theoretical gravimetric density of 10.6 wt% H2. In order to decrease the temperature where hydrogen is released, we investigated the catalytic influence of Fe2O3 on LiAlH4 dehydrogenation, as a model case for understanding the effects transition oxide additives have in the catalysis process. Quick mechanochemical synthesis of LiAlH4 + 5 wt% Fe2O3 led to the significant decrease of the hydrogen desorption temperature, and desorption of over 7 wt%H2 in the temperature range 143–154 °C. Density functional theory (DFT)-based calculations with Tran-Blaha modified Becke-Johnson functional (TBmBJ) address the electronic structure of LiAlH4 and Li3AlH6. 57Fe Mössbauer study shows the change in the oxidational state of iron during hydrogen desorption, while the 1H NMR study reveals the presence of paramagnetic species that affect relaxation. The electron transfer from hydrides is discussed as the proposed mechanism of destabilization of LiAlH4 + 5 wt% Fe2O3. © 2021 Hydrogen Energy Publications LLC T2 - International Journal of Hydrogen Energy T1 - Mechanochemical modification of LiAlH4 with Fe2O3 - A combined DFT and experimental study VL - 46 IS - 24 SP - 13070 EP - 13081 DO - 10.1016/j.ijhydene.2021.01.086 ER -
@article{ author = "Dragojlović, Milijana and Milanović, Igor and Gradišek, Anton and Kurko, Sandra V. and Mitrić, Miodrag and Umićević, Ana and Radaković, Jana and Batalović, Katarina", year = "2021", abstract = "LiAlH4 is a promising material for hydrogen storage, having the theoretical gravimetric density of 10.6 wt% H2. In order to decrease the temperature where hydrogen is released, we investigated the catalytic influence of Fe2O3 on LiAlH4 dehydrogenation, as a model case for understanding the effects transition oxide additives have in the catalysis process. Quick mechanochemical synthesis of LiAlH4 + 5 wt% Fe2O3 led to the significant decrease of the hydrogen desorption temperature, and desorption of over 7 wt%H2 in the temperature range 143–154 °C. Density functional theory (DFT)-based calculations with Tran-Blaha modified Becke-Johnson functional (TBmBJ) address the electronic structure of LiAlH4 and Li3AlH6. 57Fe Mössbauer study shows the change in the oxidational state of iron during hydrogen desorption, while the 1H NMR study reveals the presence of paramagnetic species that affect relaxation. The electron transfer from hydrides is discussed as the proposed mechanism of destabilization of LiAlH4 + 5 wt% Fe2O3. © 2021 Hydrogen Energy Publications LLC", journal = "International Journal of Hydrogen Energy", title = "Mechanochemical modification of LiAlH4 with Fe2O3 - A combined DFT and experimental study", volume = "46", number = "24", pages = "13070-13081", doi = "10.1016/j.ijhydene.2021.01.086" }
Dragojlović, M., Milanović, I., Gradišek, A., Kurko, S. V., Mitrić, M., Umićević, A., Radaković, J.,& Batalović, K.. (2021). Mechanochemical modification of LiAlH4 with Fe2O3 - A combined DFT and experimental study. in International Journal of Hydrogen Energy, 46(24), 13070-13081. https://doi.org/10.1016/j.ijhydene.2021.01.086
Dragojlović M, Milanović I, Gradišek A, Kurko SV, Mitrić M, Umićević A, Radaković J, Batalović K. Mechanochemical modification of LiAlH4 with Fe2O3 - A combined DFT and experimental study. in International Journal of Hydrogen Energy. 2021;46(24):13070-13081. doi:10.1016/j.ijhydene.2021.01.086 .
Dragojlović, Milijana, Milanović, Igor, Gradišek, Anton, Kurko, Sandra V., Mitrić, Miodrag, Umićević, Ana, Radaković, Jana, Batalović, Katarina, "Mechanochemical modification of LiAlH4 with Fe2O3 - A combined DFT and experimental study" in International Journal of Hydrogen Energy, 46, no. 24 (2021):13070-13081, https://doi.org/10.1016/j.ijhydene.2021.01.086 . .