Decomposition mechanism and the effects of metal additives on the kinetics of lithium alanate
文献信息
Anderson Janotti, Chris G. Van de Walle
First-principles density functional theory studies have been carried out for native defects and transition-metal (Ti and Ni) impurities in lithium alanate (LiAlH4), a potential material for hydrogen storage. On the basis of our detailed analysis of the structure, energetics, and migration of lithium-, aluminium-, and hydrogen-related defects, we propose a specific atomistic mechanism for the decomposition and dehydrogenation of LiAlH4 that involves mass transport mediated by native point defects. We also discuss how Ti and Ni impurities alter the Fermi-level position with respect to that in the undoped material, thus changing the concentration of charged defects that are responsible for mass transport. This mechanism provides an explanation for the experimentally observed lowering of the temperature for the onset of decomposition and of the activation energy for hydrogen desorption from LiAlH4.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










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