Na1+ xMnx/2Zr2- x/2(PO4)3as a Li+and Na+Super Ion Conductor for Solid-State Batteries

Anand Parejiya; Rachid Essehli; Ruhul Amin; Jue Liu; Nitin Muralidharan; Harry M. Meyer; David L. Wood; Ilias Belharouak

doi:10.1021/acsenergylett.0c02513

Na_{1+ x}Mn_x/2Zr_{2- x/2}(PO₄)₃as a Li⁺and Na⁺Super Ion Conductor for Solid-State Batteries

Anand Parejiya, Rachid Essehli, Ruhul Amin, Jue Liu, Nitin Muralidharan, Harry M. Meyer, David L. Wood, Ilias Belharouak

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

18 Scopus citations

Abstract

Here we report dual ion conduction capability of Na-based NASICON type super ion conductor materials using Na1+xMnx/2Zr2-x/2(PO4)3 (NMZP) as a candidate system. This method enables the use of Na-based NASICON material family in both Na as well as Li all solid-state batteries (SSBs). NZMPs with x = 1.5 and x = 2 showed the highest room-temperature conductivities of 2.86 × 10-5 and 2.82 × 10-5 S cm-1, respectively. Crystallographic analysis using neutron diffraction revealed that conductivities observed in these materials are related to the variations in the Na-O bond length and the concentration of mobile sodium content. Using galvanostatic plating and stripping tests, we show that these NMZPs boast good cycling stability against both Na and Li metals, which also reveals dual ion conduction. Mechanistic investigations through post-mortem SEM/EDS and XPS characterizations of the alkali metal and the cycled NMZPs confirm that the Na-Li ion-exchange occurs readily in these materials when electrochemically cycled.

Original language	English
Pages (from-to)	429-436
Number of pages	8
Journal	ACS Energy Letters
Volume	6
Issue number	2
DOIs	https://doi.org/10.1021/acsenergylett.0c02513
State	Published - Feb 12 2021

Funding

This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). This research at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) under contract DE-AC05-00OR22725, was sponsored by Laboratory Directed Research and Development (LDRD) Program at Oak Ridge National Laboratory, and the Office of Energy Efficiency and Renewable Energy (EERE) Vehicle Technologies Office (VTO) (Deputy Director: David Howell) Applied Battery Research subprogram (Program Manager: Peter Faguy). We also acknowledge Dr. Yaocai Bai from Oak Ridge National Laboratory for helping us with ICP-OES measurements. Research conducted at the POWGEN beamline at ORNL’s Spallation Neutron Source was sponsored by the Scientific User Facilities Division, Office of Basic Sciences, U.S. Department of Energy. A portion of this research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.

Funders	Funder number
U.S. Department of Energy
U.S. Department of Energy
Laboratory Directed Research and Development
U.S. Department of Energy
Office of Energy Efficiency and Renewable Energy
Vehicle Technologies Office
Oak Ridge National Laboratory
Office of Basic Sciences
UT-Battelle
U.S. Department of Energy	DE-AC05-00OR22725
Scientific User Facilities Division
Office of Energy Efficiency and Renewable Energy

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10.1021/acsenergylett.0c02513

Cite this

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title = "Na1+ xMnx/2Zr2- x/2(PO4)3as a Li+and Na+Super Ion Conductor for Solid-State Batteries",

abstract = "Here we report dual ion conduction capability of Na-based NASICON type super ion conductor materials using Na1+xMnx/2Zr2-x/2(PO4)3 (NMZP) as a candidate system. This method enables the use of Na-based NASICON material family in both Na as well as Li all solid-state batteries (SSBs). NZMPs with x = 1.5 and x = 2 showed the highest room-temperature conductivities of 2.86 × 10-5 and 2.82 × 10-5 S cm-1, respectively. Crystallographic analysis using neutron diffraction revealed that conductivities observed in these materials are related to the variations in the Na-O bond length and the concentration of mobile sodium content. Using galvanostatic plating and stripping tests, we show that these NMZPs boast good cycling stability against both Na and Li metals, which also reveals dual ion conduction. Mechanistic investigations through post-mortem SEM/EDS and XPS characterizations of the alkali metal and the cycled NMZPs confirm that the Na-Li ion-exchange occurs readily in these materials when electrochemically cycled.",

author = "Anand Parejiya and Rachid Essehli and Ruhul Amin and Jue Liu and Nitin Muralidharan and Meyer, {Harry M.} and Wood, {David L.} and Ilias Belharouak",

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AU - Parejiya, Anand

AU - Essehli, Rachid

AU - Amin, Ruhul

AU - Liu, Jue

AU - Muralidharan, Nitin

AU - Meyer, Harry M.

AU - Wood, David L.

AU - Belharouak, Ilias

PY - 2021/2/12

Y1 - 2021/2/12

N2 - Here we report dual ion conduction capability of Na-based NASICON type super ion conductor materials using Na1+xMnx/2Zr2-x/2(PO4)3 (NMZP) as a candidate system. This method enables the use of Na-based NASICON material family in both Na as well as Li all solid-state batteries (SSBs). NZMPs with x = 1.5 and x = 2 showed the highest room-temperature conductivities of 2.86 × 10-5 and 2.82 × 10-5 S cm-1, respectively. Crystallographic analysis using neutron diffraction revealed that conductivities observed in these materials are related to the variations in the Na-O bond length and the concentration of mobile sodium content. Using galvanostatic plating and stripping tests, we show that these NMZPs boast good cycling stability against both Na and Li metals, which also reveals dual ion conduction. Mechanistic investigations through post-mortem SEM/EDS and XPS characterizations of the alkali metal and the cycled NMZPs confirm that the Na-Li ion-exchange occurs readily in these materials when electrochemically cycled.

AB - Here we report dual ion conduction capability of Na-based NASICON type super ion conductor materials using Na1+xMnx/2Zr2-x/2(PO4)3 (NMZP) as a candidate system. This method enables the use of Na-based NASICON material family in both Na as well as Li all solid-state batteries (SSBs). NZMPs with x = 1.5 and x = 2 showed the highest room-temperature conductivities of 2.86 × 10-5 and 2.82 × 10-5 S cm-1, respectively. Crystallographic analysis using neutron diffraction revealed that conductivities observed in these materials are related to the variations in the Na-O bond length and the concentration of mobile sodium content. Using galvanostatic plating and stripping tests, we show that these NMZPs boast good cycling stability against both Na and Li metals, which also reveals dual ion conduction. Mechanistic investigations through post-mortem SEM/EDS and XPS characterizations of the alkali metal and the cycled NMZPs confirm that the Na-Li ion-exchange occurs readily in these materials when electrochemically cycled.

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