Structural Stabilization of P2-type Sodium Iron Manganese Oxides by Electrochemically Inactive Mg Substitution: Insights of Redox Behavior and Voltage Decay

Junghoon Yang; Annalise E. Maughan; Glenn Teeter; Bertrand J. Tremolet de Villers; Seong Min Bak; Sang Don Han

doi:10.1002/cssc.202001963

Structural Stabilization of P2-type Sodium Iron Manganese Oxides by Electrochemically Inactive Mg Substitution: Insights of Redox Behavior and Voltage Decay

Junghoon Yang, Annalise E. Maughan, Glenn Teeter, Bertrand J. Tremolet de Villers, Seong Min Bak, Sang Don Han

Department of Materials Science and Engineering

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

Abstract

Layered P2-type Na_0.8Mn_0.5Fe_0.5O₂ cathode material is a promising candidate for next-generation sodium-ion batteries due to the economical and environmentally benign characteristics of Mn and Fe. The poor cycling stability of the material, however, is still a problem that must be solved. To address the problem, electrochemically inactive Mg²⁺ was introduced into the structure by substituting some of the Fe ions. It was shown that Mg substitution led to a smoother voltage profile with improved cycling performance and rate capability. These observations were attributed to the suppressed structural changes during electrochemical processes. Detailed redox mechanisms, associated local structural changes, and phase transitions were investigated by X-ray absorption spectroscopy and X-ray diffraction. From the detailed analysis of electrochemical behaviors, it was also identified how the redox reactions and structural disordering occurred in the high- and low-voltage regions and how Mg substitution stabilized the structure.

Original language	English
Pages (from-to)	5972-5982
Number of pages	11
Journal	ChemSusChem
Volume	13
Issue number	22
DOIs	https://doi.org/10.1002/cssc.202001963
Publication status	Published - 2020 Nov 20

Bibliographical note

Funding Information:
This work was authored in part by Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract No. DE‐AC36‐08GO28308. Funding for material synthesis, XRD, XPS, and electrochemical characterization provided by the Laboratory Directed Research and Development program. XAS support and analysis performed at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE through the Advanced Battery Materials Research (BMR) Program under Contract No. DE‐SC0012704. The XAS research used beamline 7‐BM (QAS) of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government.

Publisher Copyright:
© 2020 Wiley-VCH GmbH

All Science Journal Classification (ASJC) codes

Environmental Chemistry
Chemical Engineering(all)
Materials Science(all)
Energy(all)

Access to Document

10.1002/cssc.202001963

Cite this

@article{82b8f5e4a4d342ffbc29c536a7e3f68a,

title = "Structural Stabilization of P2-type Sodium Iron Manganese Oxides by Electrochemically Inactive Mg Substitution: Insights of Redox Behavior and Voltage Decay",

abstract = "Layered P2-type Na0.8Mn0.5Fe0.5O2 cathode material is a promising candidate for next-generation sodium-ion batteries due to the economical and environmentally benign characteristics of Mn and Fe. The poor cycling stability of the material, however, is still a problem that must be solved. To address the problem, electrochemically inactive Mg2+ was introduced into the structure by substituting some of the Fe ions. It was shown that Mg substitution led to a smoother voltage profile with improved cycling performance and rate capability. These observations were attributed to the suppressed structural changes during electrochemical processes. Detailed redox mechanisms, associated local structural changes, and phase transitions were investigated by X-ray absorption spectroscopy and X-ray diffraction. From the detailed analysis of electrochemical behaviors, it was also identified how the redox reactions and structural disordering occurred in the high- and low-voltage regions and how Mg substitution stabilized the structure.",

author = "Junghoon Yang and Maughan, {Annalise E.} and Glenn Teeter and {Tremolet de Villers}, {Bertrand J.} and Bak, {Seong Min} and Han, {Sang Don}",

note = "Funding Information: This work was authored in part by Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract No. DE‐AC36‐08GO28308. Funding for material synthesis, XRD, XPS, and electrochemical characterization provided by the Laboratory Directed Research and Development program. XAS support and analysis performed at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE through the Advanced Battery Materials Research (BMR) Program under Contract No. DE‐SC0012704. The XAS research used beamline 7‐BM (QAS) of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. Publisher Copyright: {\textcopyright} 2020 Wiley-VCH GmbH",

year = "2020",

month = nov,

day = "20",

doi = "10.1002/cssc.202001963",

language = "English",

volume = "13",

pages = "5972--5982",

journal = "ChemSusChem",

issn = "1864-5631",

publisher = "Wiley-VCH Verlag",

number = "22",

}

TY - JOUR

T1 - Structural Stabilization of P2-type Sodium Iron Manganese Oxides by Electrochemically Inactive Mg Substitution

T2 - Insights of Redox Behavior and Voltage Decay

AU - Yang, Junghoon

AU - Maughan, Annalise E.

AU - Teeter, Glenn

AU - Tremolet de Villers, Bertrand J.

AU - Bak, Seong Min

AU - Han, Sang Don

N1 - Funding Information: This work was authored in part by Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory for the U.S. Department of Energy (DOE) under Contract No. DE‐AC36‐08GO28308. Funding for material synthesis, XRD, XPS, and electrochemical characterization provided by the Laboratory Directed Research and Development program. XAS support and analysis performed at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. DOE through the Advanced Battery Materials Research (BMR) Program under Contract No. DE‐SC0012704. The XAS research used beamline 7‐BM (QAS) of the National Synchrotron Light Source II, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. Publisher Copyright: © 2020 Wiley-VCH GmbH

PY - 2020/11/20

Y1 - 2020/11/20

N2 - Layered P2-type Na0.8Mn0.5Fe0.5O2 cathode material is a promising candidate for next-generation sodium-ion batteries due to the economical and environmentally benign characteristics of Mn and Fe. The poor cycling stability of the material, however, is still a problem that must be solved. To address the problem, electrochemically inactive Mg2+ was introduced into the structure by substituting some of the Fe ions. It was shown that Mg substitution led to a smoother voltage profile with improved cycling performance and rate capability. These observations were attributed to the suppressed structural changes during electrochemical processes. Detailed redox mechanisms, associated local structural changes, and phase transitions were investigated by X-ray absorption spectroscopy and X-ray diffraction. From the detailed analysis of electrochemical behaviors, it was also identified how the redox reactions and structural disordering occurred in the high- and low-voltage regions and how Mg substitution stabilized the structure.

AB - Layered P2-type Na0.8Mn0.5Fe0.5O2 cathode material is a promising candidate for next-generation sodium-ion batteries due to the economical and environmentally benign characteristics of Mn and Fe. The poor cycling stability of the material, however, is still a problem that must be solved. To address the problem, electrochemically inactive Mg2+ was introduced into the structure by substituting some of the Fe ions. It was shown that Mg substitution led to a smoother voltage profile with improved cycling performance and rate capability. These observations were attributed to the suppressed structural changes during electrochemical processes. Detailed redox mechanisms, associated local structural changes, and phase transitions were investigated by X-ray absorption spectroscopy and X-ray diffraction. From the detailed analysis of electrochemical behaviors, it was also identified how the redox reactions and structural disordering occurred in the high- and low-voltage regions and how Mg substitution stabilized the structure.

UR - http://www.scopus.com/inward/record.url?scp=85092096456&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85092096456&partnerID=8YFLogxK

U2 - 10.1002/cssc.202001963

DO - 10.1002/cssc.202001963

M3 - Article

C2 - 32985100

AN - SCOPUS:85092096456

SN - 1864-5631

VL - 13

SP - 5972

EP - 5982

JO - ChemSusChem

JF - ChemSusChem

IS - 22

ER -

Structural Stabilization of P2-type Sodium Iron Manganese Oxides by Electrochemically Inactive Mg Substitution: Insights of Redox Behavior and Voltage Decay

Abstract

Bibliographical note

All Science Journal Classification (ASJC) codes

Access to Document

Other files and links

Fingerprint

Cite this