.png){kind=icon}
.png){kind=icon}
Return
First-principles calculated decomposition pathways for LiBH4 nanoclusters
.png){kind=icon}
OA
AI
DOI：10.1038/srep26056.png)
.png){kind=icon}
.png){kind=icon}
Share.png){kind=icon}
Save
Abstract
En 中文
We analyze thermodynamic stability and decomposition pathways of LiBH4 nanoclusters using grand-canonical free-energy minimization based on total energies and vibrational frequencies obtained from density-functional theory (DFT) calculations. We consider (LiBH4)(n) nanoclusters with n = 2 to 12 as reactants, while the possible products include (Li)(n), (B)(n), (LiB)(n), (LiH)(n), and Li2BnHn; off-stoichiometric LinBnHm (m <= 4n) clusters were considered for n = 2, 3, and 6. Cluster ground-state configurations have been predicted using prototype electrostatic ground-state (PEGS) and genetic algorithm (GA) based structural optimizations. Free-energy calculations show hydrogen release pathways markedly differ from those in bulk LiBH4. While experiments have found that the bulk material decomposes into LiH and B, with Li2B12H12 as a kinetically inhibited intermediate phase, (LiBH4)(n) nanoclusters with n = 12 are predicted to decompose into mixed LinBn clusters via a series of intermediate clusters of LinBnHm (m = 4n). The calculated pressure-composition isotherms and temperature-pressure isobars exhibit sloping plateaus due to finite size effects on reaction thermodynamics. Generally, decomposition temperatures of free-standing clusters are found to increase with decreasing cluster size due to thermodynamic destabilization of reaction products.
Keywords:
HYDROGEN RELEASE
B-N
STORAGE
DESTABILIZATION
CARBON
DEHYDROGENATION
REVERSIBILITY
DESORPTION
STABILITY
MAGNESIUM
AI Summary
Key information extracted from the uploaded paper, including a brief overview, abstract, background, key highlights, visual analysis, and future outlook.
Journal
IF:
3.9
Papers:
27.8W
Citations:
83.5W
