Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 31, Pages 9823-9827Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201805753
Keywords
chemical bonding; hydrogen; hydrogen storage; palladium; solid-state chemistry
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Funding
- Core Research for Evolutional Science and Technology (CREST) from the Japan Science and Technology Agency (JST), Japan [JPMJAC1501]
- ACCEL from the Japan Science and Technology Agency (JST), Japan [JPMJAC1501]
- JSPS KAKENHI, Japan [16H06519, 15J01605]
- Grants-in-Aid for Scientific Research [15J01605, 16H06519] Funding Source: KAKEN
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The palladium-hydrogen system is one of the most famous hydrogen-storage systems. Although there has been much research on -phase PdH(D)(x), we comprehensively investigated the nature of the interaction between Pd and H(D) in -phase PdH(D)(x) (x<0.03 at 303K), and revealed the existence of Pd-H(D) chemical bond for the first time, by various insitu experimental techniques and first-principles theoretical calculations. The lattice expansion, magnetic susceptibility, and electrical resistivity all provide evidence. Insitu solid-state H-1 and (HNMR)-H-2 spectroscopy and first-principles theoretical calculations revealed that a Pd-H(D) chemical bond exists in the phase, but the bonding character of the Pd-H(D) bond in the phase is quite different from that in the phase; the nature of the Pd-H(D) bond in the phase is a localized covalent bond whereas that in the phase is a metallic bond.
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