Elevating Energy Density for Sodium-Ion Batteries through Multielectron Reactions

Yongjie Zhao; Xiangwen Gao; Hongcai Gao; Andrei Dolocan; John B. Goodenough

doi:10.1021/acs.nanolett.1c00100

Elevating Energy Density for Sodium-Ion Batteries through Multielectron Reactions

Yongjie Zhao^*, Xiangwen Gao^*, Hongcai Gao, Andrei Dolocan, John B. Goodenough

^*Corresponding author for this work

School of Material Science and Engineering

University of Texas at Austin

Research output: Contribution to journal › Article › peer-review

71 Citations (Scopus)

Abstract

It remains a great challenge to explore desirable cathodes for sodium-ion batteries to satisfy the ever-increasing demand for large-scale energy storage systems. In this Letter, we report a NASICON-structured Na4MnCr(PO4)3 cathode with high specific capacity and operation potential. The reversible access of the Mn2+/Mn3+ (3.75/3.4 V), Mn3+/Mn4+ (4.25/4.1 V), and Cr3+/Cr4+ (4.4/4.3 V vs Na/Na+) redox couples in a Na4MnCr(PO4)3 cathode endows a distinct three-electron redox reaction during the insertion/extraction process. The highly stable NASICON structure with a small volume variation upon cycling ensures long-time cycling stability (73.3% capacity retention after 500 cycles within the potential region of 2.5-4.6 V). The impedance analysis and interface characterization indicate that the evolution of a cathode electrolyte interphase at high potential is correlated with the capacity fading, while the robustness of the NASICON framework is redemonstrated.

Original language	English
Pages (from-to)	2281-2287
Number of pages	7
Journal	Nano Letters
Volume	21
Issue number	5
DOIs	https://doi.org/10.1021/acs.nanolett.1c00100
Publication status	Published - 10 Mar 2021

Keywords

cathode electrolyte interphase
high voltage cathode
multielectron reaction
sodium-ion batteries

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title = "Elevating Energy Density for Sodium-Ion Batteries through Multielectron Reactions",

abstract = "It remains a great challenge to explore desirable cathodes for sodium-ion batteries to satisfy the ever-increasing demand for large-scale energy storage systems. In this Letter, we report a NASICON-structured Na4MnCr(PO4)3 cathode with high specific capacity and operation potential. The reversible access of the Mn2+/Mn3+ (3.75/3.4 V), Mn3+/Mn4+ (4.25/4.1 V), and Cr3+/Cr4+ (4.4/4.3 V vs Na/Na+) redox couples in a Na4MnCr(PO4)3 cathode endows a distinct three-electron redox reaction during the insertion/extraction process. The highly stable NASICON structure with a small volume variation upon cycling ensures long-time cycling stability (73.3% capacity retention after 500 cycles within the potential region of 2.5-4.6 V). The impedance analysis and interface characterization indicate that the evolution of a cathode electrolyte interphase at high potential is correlated with the capacity fading, while the robustness of the NASICON framework is redemonstrated.",

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author = "Yongjie Zhao and Xiangwen Gao and Hongcai Gao and Andrei Dolocan and Goodenough, {John B.}",

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AU - Dolocan, Andrei

AU - Goodenough, John B.

PY - 2021/3/10

Y1 - 2021/3/10

N2 - It remains a great challenge to explore desirable cathodes for sodium-ion batteries to satisfy the ever-increasing demand for large-scale energy storage systems. In this Letter, we report a NASICON-structured Na4MnCr(PO4)3 cathode with high specific capacity and operation potential. The reversible access of the Mn2+/Mn3+ (3.75/3.4 V), Mn3+/Mn4+ (4.25/4.1 V), and Cr3+/Cr4+ (4.4/4.3 V vs Na/Na+) redox couples in a Na4MnCr(PO4)3 cathode endows a distinct three-electron redox reaction during the insertion/extraction process. The highly stable NASICON structure with a small volume variation upon cycling ensures long-time cycling stability (73.3% capacity retention after 500 cycles within the potential region of 2.5-4.6 V). The impedance analysis and interface characterization indicate that the evolution of a cathode electrolyte interphase at high potential is correlated with the capacity fading, while the robustness of the NASICON framework is redemonstrated.

AB - It remains a great challenge to explore desirable cathodes for sodium-ion batteries to satisfy the ever-increasing demand for large-scale energy storage systems. In this Letter, we report a NASICON-structured Na4MnCr(PO4)3 cathode with high specific capacity and operation potential. The reversible access of the Mn2+/Mn3+ (3.75/3.4 V), Mn3+/Mn4+ (4.25/4.1 V), and Cr3+/Cr4+ (4.4/4.3 V vs Na/Na+) redox couples in a Na4MnCr(PO4)3 cathode endows a distinct three-electron redox reaction during the insertion/extraction process. The highly stable NASICON structure with a small volume variation upon cycling ensures long-time cycling stability (73.3% capacity retention after 500 cycles within the potential region of 2.5-4.6 V). The impedance analysis and interface characterization indicate that the evolution of a cathode electrolyte interphase at high potential is correlated with the capacity fading, while the robustness of the NASICON framework is redemonstrated.

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KW - high voltage cathode

KW - multielectron reaction

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ER -

Elevating Energy Density for Sodium-Ion Batteries through Multielectron Reactions

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Keywords

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