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The Electronic State of Hydrogen in the α Phase of the Hydrogen‐Storage Material PdH(D) x : Does a Chemical Bond Between Palladium and Hydrogen Exist?
Author(s) -
Dekura Shun,
Kobayashi Hirokazu,
Ikeda Ryuichi,
Maesato Mitsuhiko,
Yoshino Haruka,
Ohba Masaaki,
Ishimoto Takayoshi,
Kawaguchi Shogo,
Kubota Yoshiki,
Yoshioka Satoru,
Matsumura Syo,
Sugiyama Takeharu,
Kitagawa Hiroshi
Publication year - 2018
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201805753
Subject(s) - palladium , chemical bond , covalent bond , hydrogen , phase (matter) , hydrogen bond , chemistry , hydrogen storage , bond order , crystallography , materials science , bond length , crystal structure , molecule , catalysis , organic chemistry
Abstract The palladium–hydrogen system is one of the most famous hydrogen‐storage systems. Although there has been much research on β‐phase PdH(D) x , we comprehensively investigated the nature of the interaction between Pd and H(D) in α‐phase PdH(D) x ( x <0.03 at 303 K), and revealed the existence of Pd−H(D) chemical bond for the first time, by various in situ experimental techniques and first‐principles theoretical calculations. The lattice expansion, magnetic susceptibility, and electrical resistivity all provide evidence. In situ solid‐state 1 H and 2 H NMR spectroscopy and first‐principles theoretical calculations revealed that a Pd−H(D) chemical bond exists in the α phase, but the bonding character of the Pd−H(D) bond in the α phase is quite different from that in the β phase; the nature of the Pd−H(D) bond in the α phase is a localized covalent bond whereas that in the β phase is a metallic bond.