TY - JOUR
T1 - The role of A-site ion on proton diffusion in perovskite oxides (ABO3)
AU - Jing, Yuhang
AU - Aluru, N. R.
N1 - Funding Information:
This work is supported by the National Science Foundation under grant # 1545907 , the National Center for Supercomputing Applications (NCSA) , the NSF of China under Grant No. 11932005 and 11432005 , and the International Postdoctoral Exchange Fellowship Program of China under Grants No. 20140016 . This research is part of the Blue Waters sustained-petascale computing project, which is supported by the National Science Foundation (awards OCI-0725070 and ACI-1238993 ) and the state of Illinois. Blue Waters is a joint effort of the University of Illinois at Urbana-Champaign. The authors also acknowledge the use of the Extreme Science and Engineering Discovery Environment (XSEDE). Appendix A
Funding Information:
This work is supported by the National Science Foundation under grant # 1545907, the National Center for Supercomputing Applications (NCSA), the NSF of China under Grant No. 11932005 and 11432005, and the International Postdoctoral Exchange Fellowship Program of China under Grants No. 20140016. This research is part of the Blue Waters sustained-petascale computing project, which is supported by the National Science Foundation (awards OCI-0725070 and ACI-1238993) and the state of Illinois. Blue Waters is a joint effort of the University of Illinois at Urbana-Champaign. The authors also acknowledge the use of the Extreme Science and Engineering Discovery Environment (XSEDE).
Publisher Copyright:
© 2019 Elsevier B.V.
PY - 2020/1/1
Y1 - 2020/1/1
N2 - By performing detailed density functional theory (DFT) calculations, we investigate the effect of A ion vacancy on both hydroxide ion rotation and proton transfer in Y-doped BaZrO3. We find that A ions reduce the barrier for proton diffusion in a perovskite oxide, demonstrating the significance of perovskite structures as proton conductors. Proton diffusion is understood as a two-step mechanism consisting of hydroxide ion rotation and proton transfer. In both steps, lattice deformations play an important role – specifically, the outward O-B-O bending and A ion motions are important for hydroxide ion rotation, and inward O-B-O bending facilitates proton transfer. By comparing the bond strength, we reveal that an A ion can reduce the bond strength of O and B ion, thereby reducing the energy barrier for local lattice deformation such as O-B-O bending motion, which facilitates both hydroxide ion rotation and proton transfer. Our analysis provides a detailed atomistic understanding of the role of A-site ion on proton diffusion in perovskite oxides. The study presented here not only indicates the advantage of perovskite oxides as proton conductors but also elucidates the origin of proton diffusion barrier which can pave the way for design of novel proton conductors.
AB - By performing detailed density functional theory (DFT) calculations, we investigate the effect of A ion vacancy on both hydroxide ion rotation and proton transfer in Y-doped BaZrO3. We find that A ions reduce the barrier for proton diffusion in a perovskite oxide, demonstrating the significance of perovskite structures as proton conductors. Proton diffusion is understood as a two-step mechanism consisting of hydroxide ion rotation and proton transfer. In both steps, lattice deformations play an important role – specifically, the outward O-B-O bending and A ion motions are important for hydroxide ion rotation, and inward O-B-O bending facilitates proton transfer. By comparing the bond strength, we reveal that an A ion can reduce the bond strength of O and B ion, thereby reducing the energy barrier for local lattice deformation such as O-B-O bending motion, which facilitates both hydroxide ion rotation and proton transfer. Our analysis provides a detailed atomistic understanding of the role of A-site ion on proton diffusion in perovskite oxides. The study presented here not only indicates the advantage of perovskite oxides as proton conductors but also elucidates the origin of proton diffusion barrier which can pave the way for design of novel proton conductors.
KW - Density functional theory calculation
KW - Lattice deformation
KW - Origin of energy barrier
KW - Perovskite oxide
KW - Proton diffusion
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U2 - 10.1016/j.jpowsour.2019.227327
DO - 10.1016/j.jpowsour.2019.227327
M3 - Article
AN - SCOPUS:85073675774
VL - 445
JO - Journal of Power Sources
JF - Journal of Power Sources
SN - 0378-7753
M1 - 227327
ER -