Discrete Li-occupation versus pseudo-continuous Na-occupation and their relationship with structural change behaviors in Fe2(MoO4)3.
The key factors governing the single-phase or multi-phase structural change behaviors during the intercalation/deintercalation of guest ions have not been well studied and understood yet. Through systematic studies of orthorhombic Fe2(MoO4)3 electrode, two distinct guest ion occupation paths, namely discrete one for Li and pseudo-continuous one for Na, as well as their relationship with single-phase and two-phase modes for Na(+) and Li(+), respectively during the intercalation/deintercalation process have been demonstrated. For the first time, the direct atomic-scale observation of biphasic domains (discrete occupation) in partially lithiated Fe2(MoO4)3 and the one by one Na occupation (pseudo-continuous occupation) at 8d sites in partially sodiated Fe2(MoO4)3 are obtained during the discharge processes of Li/Fe2(MoO4)3 and Na/Fe2(MoO4)3 cells respectively. Our combined experimental and theoretical studies bring the new insights for the research and development of intercalation compounds as electrode materials for secondary batteries.
Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials, Department of Chemistry &Laser Chemistry Institute, Fudan University, Shanghai 200433, P.R. China.
Ji-Li
JL
Yue
Departmentof Chemistry, Brookhaven National Laboratory, Upton, New York 11973, USA.
Yong-Ning
YN
Zhou
School of Materials Science and Engineering, Shanghai University, Shanghai 200444, P.R. China.
Si-Qi
SQ
Shi
Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials, Department of Chemistry &Laser Chemistry Institute, Fudan University, Shanghai 200433, P.R. China.
Zulipiya
Z
Shadike
Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials, Department of Chemistry &Laser Chemistry Institute, Fudan University, Shanghai 200433, P.R. China.
Xuan-Qi
XQ
Huang
School of Materials Science and Engineering, Shanghai University, Shanghai 200444, P.R. China.
Jun
J
Luo
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, PO Box 603, Beijing 100190, P.R. China.
Zhen-Zhong
ZZ
Yang
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, PO Box 603, Beijing 100190, P.R. China.
Hong
H
Li
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, PO Box 603, Beijing 100190, P.R. China.
Lin
L
Gu
Departmentof Chemistry, Brookhaven National Laboratory, Upton, New York 11973, USA.
Xiao-Qing
XQ
Yang
Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials, Department of Chemistry &Laser Chemistry Institute, Fudan University, Shanghai 200433, P.R. China.
Zheng-Wen
ZW
Fu