Quantum‒Chemical Simulation of Molecular Hydrogen Abstraction from Magnesium Borohydride Diammoniate

Мұқаба

Дәйексөз келтіру

Толық мәтін

Ашық рұқсат Ашық рұқсат
Рұқсат жабық Рұқсат берілді
Рұқсат жабық Тек жазылушылар үшін

Аннотация

Within the framework of the cluster approach using the 6‒31G* basis set and the hybrid density functional (B3LYP), we modeled successive abstraction of H2 from the complexes (Mg(BH4)2∙2NH3)2 and (Mg(BH4)2∙2NH3)4. It was found that the initial stage of dehydrogenation needs overcoming energy barriers ~ 1.5‒1.2 eV, which requires preheating, then the process can go on with energy release until about 10 wt % of H2 is extracted, for a higher degree of conversion, additional energy costs exceeding the combustion heat of H2 will be required when extracting more than 12.5 wt % of H2. Therefore, further dehydrogenation of this compound may turn out to be inexpedient from the energy point of view.

Толық мәтін

Рұқсат жабық

Авторлар туралы

A. Zyubin

Federal Research Center for Problems of Chemical Physics and Medicinal Chemistry, Russian Academy of Sciences

Хат алмасуға жауапты Автор.
Email: zyubin@icp.ac.ru
Ресей, Chernogolovka, 142432

T. Zyubina

Federal Research Center for Problems of Chemical Physics and Medicinal Chemistry, Russian Academy of Sciences

Email: zyubin@icp.ac.ru
Ресей, Chernogolovka, 142432

O. Kravchenko

Federal Research Center for Problems of Chemical Physics and Medicinal Chemistry, Russian Academy of Sciences

Email: zyubin@icp.ac.ru
Ресей, Chernogolovka, 142432

M. Solov’ev

Federal Research Center for Problems of Chemical Physics and Medicinal Chemistry, Russian Academy of Sciences

Email: zyubin@icp.ac.ru
Ресей, Chernogolovka, 142432

V. Vasiliev

Federal Research Center for Problems of Chemical Physics and Medicinal Chemistry, Russian Academy of Sciences

Email: zyubin@icp.ac.ru
Ресей, Chernogolovka, 142432

A. Zaitsev

Federal Research Center for Problems of Chemical Physics and Medicinal Chemistry, Russian Academy of Sciences

Email: zyubin@icp.ac.ru
Ресей, Chernogolovka, 142432

A. Shikhovtsev

Federal Research Center for Problems of Chemical Physics and Medicinal Chemistry, Russian Academy of Sciences; Hydrogen energy center of AFK “Sistema”

Email: zyubin@icp.ac.ru
Ресей, Chernogolovka, 142432; Chernogolovka, 142432

Y. Dobrovol’sky

Federal Research Center for Problems of Chemical Physics and Medicinal Chemistry, Russian Academy of Sciences; Hydrogen energy center of AFK “Sistema”

Email: zyubin@icp.ac.ru
Ресей, Chernogolovka, 142432; Chernogolovka, 142432

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2. Fig. 1. Configurations of the [Mg(BH4)22NH3]2 system that occur when up to three H2 molecules are removed. The number after the letter D indicates the number of H2 molecules removed.

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3. Fig. 2. Gibbs energies for the configurations of the [Mg(BH4)22NH3]2 system arising from the removal of up to four (D0‒D4) and up to nine (D4‒D9) H2 molecules.

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4. Fig. 3. Configurations of the [Mg(BH4)22NH3]2 system that occur when four to eight H2 molecules are removed.

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5. Fig. 4. Configurations of the [Mg(BH4)22NH3]2 system that occur when eight to ten H2 molecules are removed.

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6. Fig. 5. Gibbs energies for configurations of the Mg(BH4)22NH3]2 system that occur when nine to twelve (D9‒D12) H2 molecules are removed.

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7. Fig. 6. Configurations of the [Mg(BH4)22NH3]2 system arising from the removal of eleven and twelve H2 molecules, and complexes arising from the unification of D9‒D12 structures.

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8. Fig. 7. Configurations of the [Mg(BH4)22NH3]4 system that occur when eighteen to nineteen H2 molecules are removed.

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9. Fig. 8. Configurations of the [Mg(BH4)22NH3]4 system that occur when nineteen to twenty-three H2 molecules are removed.

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10. Fig. 9. Gibbs energies for the configurations of the [Mg(BH4)22NH3]4 system arising at a distance of eighteen to twenty-three H2 molecules.

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11. Supplement
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