TY - JOUR
T1 - Complex rare-earth aluminum hydrides
T2 - Mechanochemical preparation, crystal structure and potential for hydrogen storage
AU - Weidenthaler, Claudia
AU - Pommerin, André
AU - Felderhoff, Michael
AU - Sun, Wenhao
AU - Wolverton, Christopher
AU - Bogdanović, Borislav
AU - Schüth, Ferdi
PY - 2009
Y1 - 2009
N2 - A novel type of complex rare-earth aluminum hydride was prepared by mechanochemical preparation. The crystal structure of the REAlH6 (with RE = La, Ce, Pr, Nd) compounds was calculated by DFT methods and confirmed by preliminary structure refinements. The trigonal crystal structure consists of isolated [AlH6]3- octahedra bridged via [12] coordinated RE cations. The investigation of the rare-earth aluminum hydrides during thermolysis shows a decrease of thermal stability with increasing atomic number of the RE element. Rare-earth hydrides (REHx) are formed as primary dehydrogenation products; the final products are RE-aluminum alloys. The calculated decomposition enthalpies of the rare-earth aluminum hydrides are at the lower end for reversible hydrogenation under moderate conditions. Even though these materials may require somewhat higher pressures and/or lower temperatures for rehydrogenation, they are interesting examples of low-temperature metal hydrides for which reversibility might be reached.
AB - A novel type of complex rare-earth aluminum hydride was prepared by mechanochemical preparation. The crystal structure of the REAlH6 (with RE = La, Ce, Pr, Nd) compounds was calculated by DFT methods and confirmed by preliminary structure refinements. The trigonal crystal structure consists of isolated [AlH6]3- octahedra bridged via [12] coordinated RE cations. The investigation of the rare-earth aluminum hydrides during thermolysis shows a decrease of thermal stability with increasing atomic number of the RE element. Rare-earth hydrides (REHx) are formed as primary dehydrogenation products; the final products are RE-aluminum alloys. The calculated decomposition enthalpies of the rare-earth aluminum hydrides are at the lower end for reversible hydrogenation under moderate conditions. Even though these materials may require somewhat higher pressures and/or lower temperatures for rehydrogenation, they are interesting examples of low-temperature metal hydrides for which reversibility might be reached.
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U2 - 10.1021/ja9042565
DO - 10.1021/ja9042565
M3 - Article
C2 - 19886669
AN - SCOPUS:70450191107
SN - 0002-7863
VL - 131
SP - 16735
EP - 16743
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 46
ER -