A Class of Sodium Transition‐Metal Sulfide Cathodes With Anion Redox

Author:

He Jiarui1,Bhargav Amruth1,Okasinski John2,Manthiram Arumugam1ORCID

Affiliation:

1. Materials Science and Engineering Program Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA

2. Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA

Abstract

AbstractSodium‐ion batteries (SIBs) are entering commercial relevance as a sustainable and low‐cost alternative to lithium‐ion batteries. Improving the energy density of SIBs is critical to enable their widespread adoption. Here, a new class of cathode materials Na6MS4 (M = Co, Mn, Fe, and Zn) that exhibit high charge‐storage capacity is reported. Using Na6CoS4 as a prototypical example, a six‐electron conversion reaction dominated by anion redox is observed, confirmed through various electrochemical and spectroscopic techniques. After the initial cycle, Na6CoS4 delivers a high capacity of 392 mA h g−1 with a long lifespan of over 500 cycles. The reaction involves, initially, the transformation of crystalline Na6CoS4 to a nearly amorphous structure consisting of mainly CoS and sulfur nanoparticles, which then reversibly cycles between nearly amorphous a‐CoS/S and a‐Na6CoS4. Such anion‐redox‐driven conversion‐type cathodes hold the potential to enable energy‐dense, stable SIBs.

Funder

U.S. Department of Energy

Basic Energy Sciences

Division of Materials Sciences and Engineering

Publisher

Wiley

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