Gao Peng, Huang Zhenguo, Yu Haibo
School of Chemistry and Molecular Bioscience, University of Wollongong, Wollongong, NSW 2500, Australia.
Molecular Horizons, University of Wollongong, Wollongong, NSW 2500, Australia.
J Phys Chem A. 2020 Mar 5;124(9):1698-1704. doi: 10.1021/acs.jpca.9b10441. Epub 2020 Feb 25.
Ammonium aminodiboranate (AADB) and diammoniate of diborane (DADB) are two isomers of ammonia borane (AB), which have been intensively studied for hydrogen storage. Their high hydrogen contents give them the high potential to serve as hydrogen storage materials. To explore their dehydrogenation pathways, molecular dynamics (MD) simulations with a reactive force field (ReaxFF) were applied. Temperature ramping simulations of their thermolysis were carried out. For AADB, at low temperatures, its hydrogen release can be realized mainly via intermolecular dehydrogenations. As the temperature of the simulated system increases, the formations of B-N bonds begin to occur. In the case of DADB, we found that this molecule could release hydrogen at a lower temperature with the cleavage of the B-N bond. The compositional analysis of the simulated systems was also conducted to monitor the potential intermediates along their dehydrogenation pathways. Our current work provides a detailed picture of the initial dehydrogenation steps of AADB and DADB and highlights the difference in their respective dehydrogenation processes.
氨基二硼烷铵（AADB）和乙硼烷二铵（DADB）是氨硼烷（AB）的两种异构体，它们已被深入研究用于储氢。它们的高氢含量使其具有作为储氢材料的巨大潜力。为了探索它们的脱氢途径，应用了具有反应力场（ReaxFF）的分子动力学（MD）模拟。对它们的热解进行了升温模拟。对于AADB，在低温下，其氢释放主要可通过分子间脱氢实现。随着模拟系统温度的升高，开始形成B-N键。在DADB的情况下，我们发现该分子可以在较低温度下通过B-N键的断裂释放氢。还对模拟系统进行了成分分析，以监测其脱氢途径中的潜在中间体。我们目前 的工作提供了AADB和DADB初始脱氢步骤的详细情况，并突出了它们各自脱氢过程的差异。
