Na 3 MnZr(PO 4 ) 3: A High-Voltage Cathode for Sodium Batteries

Hongcai Gao, Ieuan D. Seymour, Sen Xin, Leigang Xue, Graeme Henkelman, John B. Goodenough*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

232 Citations (Scopus)

Abstract

Sodium batteries have been regarded as promising candidates for large-scale energy storage application, provided cathode hosts with high energy density and long cycle life can be found. Herein, we report NASICON-structured Na 3 MnZr(PO 4 ) 3 as a cathode for sodium batteries that exhibits an electrochemical performance superior to those of other manganese phosphate cathodes reported in the literature. Both the Mn 4+ /Mn 3+ and Mn 3+ /Mn 2+ redox couples are reversibly accessed in Na 3 MnZr(PO 4 ) 3 , providing high discharge voltage plateaus at 4.0 and 3.5 V, respectively. A high discharge capacity of 105 mAh g -1 was obtained from Na 3 MnZr(PO 4 ) 3 with a small variation of lattice parameters and a small volume change on extraction of two Na + ions per formula unit. Moreover, Na 3 MnZr(PO 4 ) 3 exhibits an excellent cycling stability, retaining 91% of the initial capacity after 500 charge/discharge cycles at 0.5 C rate. On the basis of structural analysis and density functional theory calculations, we have proposed a detailed desodiation pathway from Na 3 MnZr(PO 4 ) 3 where Mn and Zr are disordered within the structure. We further show that the cooperative Jahn-Teller distortion of Mn 3+ is suppressed in the cathode and that Na 2 MnZr(PO 4 ) 3 is a stable phase.

Original languageEnglish
Pages (from-to)18192-18199
Number of pages8
JournalJournal of the American Chemical Society
Volume140
Issue number51
DOIs
Publication statusPublished - 26 Dec 2018
Externally publishedYes

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