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Electrochemical utilization of iron IV in the Li1.3Fe0.4Nb0.3O2 disordered rocksalt cathode

DOI: 10.1002/batt.202000318 DOI Help

Authors: Zachary W. Lebens-Higgins (Binghamton University) , Hyeseung Chung (University of California San Diego) , Israel Temprano (University of Cambridge) , Mateusz Zuba (Binghamton University) , Jinpeng Wu (Advanced Light Source) , Jatinkumar Rana (Binghamton University) , Carlos Mejia (University of California San Diego) , Michael A. Jones (University of Cambridge) , Le Wang (Pacific Northwest National Laboratory) , Clare P. Grey (University of Cambridge) , Yingge Du (Pacific Northwest National Laboratory) , Wanli Yang (Advanced Light Source) , Ying Shirley Meng (University of California San Diego) , Louis F. J. Piper (University of Warwick; Binghamton University)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Batteries & Supercaps , VOL 144

State: Published (Approved)
Published: January 2021
Diamond Proposal Number(s): 22250 , 22148

Abstract: Interest in alkali‐rich oxide cathodes has grown in an effort to identify systems that provide high energy densities through reversible oxygen redox. However, some of the most promising compositions such as those based solely on earth abundant elements, e. g., iron and manganese, suffer from poor capacity retention and large hysteresis. Here, we use the disordered rocksalt cathode, Li1.3Fe0.4Nb0.3O2, as a model system to identify the underlying origin for the poor performance of Li‐rich iron‐based cathodes. Using elementally specific spectroscopic probes, we find the first charge is primarily accounted for by iron oxidation to 4+ below 4.25 V and O2 gas release beyond 4.25 V with no evidence of bulk oxygen redox. Although the Li1.3Fe0.4Nb0.3O2 is not a viable oxygen redox cathode, the iron 3+/4+ redox couple can be used reversibly during cycling.

Journal Keywords: energy storage; Li-ion batteries; alkali-rich oxide cathodes; iron-based disordered rocksalt oxides; anionic redox

Diamond Keywords: Batteries; Lithium-ion

Subject Areas: Materials, Chemistry


Instruments: I09-Surface and Interface Structural Analysis

Other Facilities: Beamline 6BMM at National Synchrotron Light Source II (NSLS‐II)

Discipline Tags:

Energy Energy Storage Material Sciences Energy Materials Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Near Edge X-ray Absorption Fine Structures (NEXAFS)