Abstract
The exact role of catalysts, such as titanium, scandium, or cerium, in improving the hydrogen kinetics in NaAlH4 is not completely understood. Here, we studied the local structure of scandium and the formation of different species in ScCl3-doped NaAlH4 by 23Na, 27Al, and 45Sc NMR. The 27Al and 23Na solid-state NMR spectra of ball-milled ScCl3-doped NaAlH4 mainly show resonances corresponding to NaAlH4, Na3AlH6, Al, and NaCl. The three decomposition products are formed by partial dehydrogenation and reactions with the dopant. The 45Sc NMR spectrum shows resonances corresponding to a distorted ScCl3 phase, a Sc–Al solid solution, and ScH2. After cycling eight times with hydrogen, the Na3AlH6 and Al intensities increase. This can be explained by an incomplete rehydrogenation that is due to a partial reversibility of the first desorption reaction. After cycling under hydrogen, the NaCl intensity strongly increases. This indicates that the doping reaction is not completed after ball-milling. The 45Sc spectra n...
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