TY - JOUR
T1 - The Electronic State of Hydrogen in the α Phase of the Hydrogen-Storage Material PdH(D)x
T2 - Does a Chemical Bond Between Palladium and Hydrogen Exist?
AU - Dekura, Shun
AU - Kobayashi, Hirokazu
AU - Ikeda, Ryuichi
AU - Maesato, Mitsuhiko
AU - Yoshino, Haruka
AU - Ohba, Masaaki
AU - Ishimoto, Takayoshi
AU - Kawaguchi, Shogo
AU - Kubota, Yoshiki
AU - Yoshioka, Satoru
AU - Matsumura, Syo
AU - Sugiyama, Takeharu
AU - Kitagawa, Hiroshi
N1 - Funding Information:
Synchrotron in situ PXRD measurements under controllable H2 and D2 gas pressure were performed at BL02B2 in SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute (JASRI) (proposal No. 2017A1189 and 2017B1352). Synchrotron in situ XANES measurements under controllable D2 gas pressure were performed at Kyushu University Beamline (SAGA-LS/BL06), Japan (proposal No. 2017IK008). This work was supported by Core Research for Evolutional Science and Technology (CREST) and ACCEL from the Japan Science and Technology Agency (JST), Grant Number JPMJAC1501, and JSPS KAKENHI Grant Number 16H06519 (Coordination Asymmetry) and 15J01605, Japan.
Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2018/7/26
Y1 - 2018/7/26
N2 - 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 1H and 2H 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.
AB - 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 1H and 2H 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.
UR - http://www.scopus.com/inward/record.url?scp=85050469172&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85050469172&partnerID=8YFLogxK
U2 - 10.1002/anie.201805753
DO - 10.1002/anie.201805753
M3 - Article
C2 - 29896769
AN - SCOPUS:85050469172
SN - 1433-7851
VL - 57
SP - 9823
EP - 9827
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 31
ER -