Enhancing carrier transfer properties of Na-rich anti-perovskites, NaOM with tetrahedral anion groups: an evaluation through first-principles computational analysis
The practical application of Na-based solid-state electrolytes (SSEs) is limited by their low level of conduction. To evaluate the impact of tetrahedral anion groups on carrier migration, we designed a set of anti-perovskite SSEs theoretically based on the previously reported Na 4 OBr 2 , including...
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Published in | Physical chemistry chemical physics : PCCP Vol. 26; no. 25; pp. 17934 - 17943 |
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Main Authors | , , , , |
Format | Journal Article |
Published |
26.06.2024
|
Online Access | Get full text |
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Abstract | The practical application of Na-based solid-state electrolytes (SSEs) is limited by their low level of conduction. To evaluate the impact of tetrahedral anion groups on carrier migration, we designed a set of anti-perovskite SSEs theoretically based on the previously reported Na
4
OBr
2
, including Na
4
O(BH
4
)
2
, Na
4
O(BF
4
)
2
, and Na
4
O(AlH
4
)
2
. It is essential to note that the excessive radius of anionic groups inevitably leads to lattice distortion, resulting in asymmetric migration paths and a limited improvement in carrier migration rate. Na
4
O(AlH
4
)
2
provides a clear example of where Na
+
migrates in two distinct environments. In addition, due to different spatial charge distributions, the interaction strength between anionic groups and Na
+
is different. Strong interactions can cause carriers to appear on a swing, leading to a decrease in conductivity. The low conductivity of Na
4
O(BF
4
)
2
is a typical example. This study demonstrates that Na
4
O(BH
4
)
2
exhibits remarkable mechanical and dynamic stability and shows ionic conductivity of 1.09 × 10
−4
S cm
−1
, two orders of magnitude higher than that of Na
4
OBr
2
. This is attributed to the expansion of the carrier migration channels by the anion groups, the moderate interaction between carriers and anionic groups, and the "paddle-wheel" effect generated by the anion groups, indicating that the "paddle-wheel" effect is still effective in low-dimensional anti-perovskite structures, in which atoms are arranged asymmetrically.
Sodium ions migrate through migration gates (MGs) in Na
4
O(BH
4
)
2
and cause rotation of the [BH
4
]
−
clusters that make up MGs. |
---|---|
AbstractList | The practical application of Na-based solid-state electrolytes (SSEs) is limited by their low level of conduction. To evaluate the impact of tetrahedral anion groups on carrier migration, we designed a set of anti-perovskite SSEs theoretically based on the previously reported Na
4
OBr
2
, including Na
4
O(BH
4
)
2
, Na
4
O(BF
4
)
2
, and Na
4
O(AlH
4
)
2
. It is essential to note that the excessive radius of anionic groups inevitably leads to lattice distortion, resulting in asymmetric migration paths and a limited improvement in carrier migration rate. Na
4
O(AlH
4
)
2
provides a clear example of where Na
+
migrates in two distinct environments. In addition, due to different spatial charge distributions, the interaction strength between anionic groups and Na
+
is different. Strong interactions can cause carriers to appear on a swing, leading to a decrease in conductivity. The low conductivity of Na
4
O(BF
4
)
2
is a typical example. This study demonstrates that Na
4
O(BH
4
)
2
exhibits remarkable mechanical and dynamic stability and shows ionic conductivity of 1.09 × 10
−4
S cm
−1
, two orders of magnitude higher than that of Na
4
OBr
2
. This is attributed to the expansion of the carrier migration channels by the anion groups, the moderate interaction between carriers and anionic groups, and the "paddle-wheel" effect generated by the anion groups, indicating that the "paddle-wheel" effect is still effective in low-dimensional anti-perovskite structures, in which atoms are arranged asymmetrically.
Sodium ions migrate through migration gates (MGs) in Na
4
O(BH
4
)
2
and cause rotation of the [BH
4
]
−
clusters that make up MGs. |
Author | Zhao, Qinfu Zhang, Ronglan Song, Qi Xu, Shenglin Suo, Bingbing |
AuthorAffiliation | Shaanxi Key Laboratory for Theoretical Physic Frontiers Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education Northwest University Institute of Modern Physics National Demonstration Center for Experimental Chemistry Education (Northwest University) College of Chemistry and Materials Science |
AuthorAffiliation_xml | – name: Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education – name: Institute of Modern Physics – name: Northwest University – name: Shaanxi Key Laboratory for Theoretical Physic Frontiers – name: National Demonstration Center for Experimental Chemistry Education (Northwest University) – name: College of Chemistry and Materials Science |
Author_xml | – sequence: 1 givenname: Shenglin surname: Xu fullname: Xu, Shenglin – sequence: 2 givenname: Qinfu surname: Zhao fullname: Zhao, Qinfu – sequence: 3 givenname: Ronglan surname: Zhang fullname: Zhang, Ronglan – sequence: 4 givenname: Bingbing surname: Suo fullname: Suo, Bingbing – sequence: 5 givenname: Qi surname: Song fullname: Song, Qi |
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