K2Fe(C2O4)2: an oxalate cathode for Li/Na ion batteries exhibiting a combination of multielectron cation and anion redox

Atin Pramanik; Alexis G. Manche; Moulay Tahar Sougrati; Alan Chadwick; Philip Lightfoot; Robert Armstrong

doi:10.1021/acs.chemmater.3c00063

K₂Fe(C₂O₄)₂: an oxalate cathode for Li/Na ion batteries exhibiting a combination of multielectron cation and anion redox

Atin Pramanik, Alexis G. Manche, Moulay Tahar Sougrati, Alan Chadwick, Philip Lightfoot^*, Robert Armstrong^*

^*Corresponding author for this work

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

Abstract

The development of multielectron redox-active cathode materials is a top priority for achieving high energy density with long cycle life in the next-generation secondary battery applications. Triggering anion redox activity is regarded as a promising strategy to enhance the energy density of polyanionic cathodes for Li/Na-ion batteries. Herein, K₂Fe(C₂O₄)₂ is shown to be a promising new cathode material that combines metal redox activity with oxalate anion (C₂O₄^2–) redox. This compound reveals specific discharge capacities of 116 and 60 mAh g^–1 for sodium-ion batterie (NIB) and lithium-ion batterie (LIB) cathode applications, respectively, at a rate of 10 mA g^–1, with excellent cycling stability. The experimental results are complemented by density functional theory (DFT) calculations of the average atomic charges.

Original language	English
Pages (from-to)	2600-2611
Number of pages	12
Journal	Chemistry of Materials
Volume	35
Issue number	6
Early online date	13 Mar 2023
DOIs	https://doi.org/10.1021/acs.chemmater.3c00063
Publication status	Published - 28 Mar 2023

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10.1021/acs.chemmater.3c00063Licence: CC BY

Pramanik_2023_CM_Oxalatecathode_CC
Copyright © 2023 The Authors. Published by American Chemical Society. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
Final published version, 7.33 MBLicence: CC BY

Light Element Analysis Facility (LEAF): Light Element Analysis Facility (LEAF)
Irvine, J. T. S. (PI), Baker, R. (CoI) & Miller, D. N. (CoI)
EPSRC
5/04/20 → 4/04/23
Project: Standard
Electon Microscopy: Electon Microscopy for the characterisation and manipulation of advanced function materials and their interfaces at the nanoscale
Irvine, J. T. S. (PI), Baker, R. (CoI) & Zhou, W. (CoI)
EPSRC
1/04/18 → 2/09/20
Project: Standard

Cite this

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title = "K2Fe(C2O4)2: an oxalate cathode for Li/Na ion batteries exhibiting a combination of multielectron cation and anion redox",

abstract = "The development of multielectron redox-active cathode materials is a top priority for achieving high energy density with long cycle life in the next-generation secondary battery applications. Triggering anion redox activity is regarded as a promising strategy to enhance the energy density of polyanionic cathodes for Li/Na-ion batteries. Herein, K2Fe(C2O4)2 is shown to be a promising new cathode material that combines metal redox activity with oxalate anion (C2O42–) redox. This compound reveals specific discharge capacities of 116 and 60 mAh g–1 for sodium-ion batterie (NIB) and lithium-ion batterie (LIB) cathode applications, respectively, at a rate of 10 mA g–1, with excellent cycling stability. The experimental results are complemented by density functional theory (DFT) calculations of the average atomic charges.",

author = "Atin Pramanik and Manche, {Alexis G.} and Sougrati, {Moulay Tahar} and Alan Chadwick and Philip Lightfoot and Robert Armstrong",

note = "Funding: The authors thank the EPSRC for financial support (EP/R030472/1). A.G.M. thanks the Faraday Institution for financial support and training (grant number FITG033). A.R.A. thanks the Faraday Institution for financial support (FIRG018). The authors are grateful for the provision of beam time on B18 at the Diamond Light Source (as part of the Energy Materials Block Allocation Group SP25120). The authors also would like to acknowledge the EPSRC Light Element Analysis Facility Grant EP/T019298/1 and the EPSRC Strategic Equipment Resource Grant EP/R023751/1.",

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language = "English",

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AU - Pramanik, Atin

AU - Manche, Alexis G.

AU - Sougrati, Moulay Tahar

AU - Chadwick, Alan

AU - Lightfoot, Philip

AU - Armstrong, Robert

N1 - Funding: The authors thank the EPSRC for financial support (EP/R030472/1). A.G.M. thanks the Faraday Institution for financial support and training (grant number FITG033). A.R.A. thanks the Faraday Institution for financial support (FIRG018). The authors are grateful for the provision of beam time on B18 at the Diamond Light Source (as part of the Energy Materials Block Allocation Group SP25120). The authors also would like to acknowledge the EPSRC Light Element Analysis Facility Grant EP/T019298/1 and the EPSRC Strategic Equipment Resource Grant EP/R023751/1.

PY - 2023/3/28

Y1 - 2023/3/28

N2 - The development of multielectron redox-active cathode materials is a top priority for achieving high energy density with long cycle life in the next-generation secondary battery applications. Triggering anion redox activity is regarded as a promising strategy to enhance the energy density of polyanionic cathodes for Li/Na-ion batteries. Herein, K2Fe(C2O4)2 is shown to be a promising new cathode material that combines metal redox activity with oxalate anion (C2O42–) redox. This compound reveals specific discharge capacities of 116 and 60 mAh g–1 for sodium-ion batterie (NIB) and lithium-ion batterie (LIB) cathode applications, respectively, at a rate of 10 mA g–1, with excellent cycling stability. The experimental results are complemented by density functional theory (DFT) calculations of the average atomic charges.

AB - The development of multielectron redox-active cathode materials is a top priority for achieving high energy density with long cycle life in the next-generation secondary battery applications. Triggering anion redox activity is regarded as a promising strategy to enhance the energy density of polyanionic cathodes for Li/Na-ion batteries. Herein, K2Fe(C2O4)2 is shown to be a promising new cathode material that combines metal redox activity with oxalate anion (C2O42–) redox. This compound reveals specific discharge capacities of 116 and 60 mAh g–1 for sodium-ion batterie (NIB) and lithium-ion batterie (LIB) cathode applications, respectively, at a rate of 10 mA g–1, with excellent cycling stability. The experimental results are complemented by density functional theory (DFT) calculations of the average atomic charges.

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DO - 10.1021/acs.chemmater.3c00063

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VL - 35

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JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 6

ER -

K2Fe(C2O4)2: an oxalate cathode for Li/Na ion batteries exhibiting a combination of multielectron cation and anion redox

Abstract

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Light Element Analysis Facility (LEAF): Light Element Analysis Facility (LEAF)

Electon Microscopy: Electon Microscopy for the characterisation and manipulation of advanced function materials and their interfaces at the nanoscale

Cite this

K₂Fe(C₂O₄)₂: an oxalate cathode for Li/Na ion batteries exhibiting a combination of multielectron cation and anion redox