Journal of the American Chemical Society, volume 141, issue 48, pages 19002-19013

New Family of Argyrodite Thioantimonate Lithium Superionic Conductors

Laidong Zhou ¹

Abdeljalil Assoud ¹

Vijay Kumar Singh ²

Xiaohan Wu ³

Linda F. Nazar ¹

Hide authors affiliations Show authors affiliations: 3 affiliations

Department of Chemistry and the Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Avenue West, Waterloo, Ontario N2L 3G1, Canada |

Neutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States |

BASF SE, Ludwigshafen 67056, Germany |

Publication type: Journal Article

Publication date: 2019-10-23

American Chemical Society (ACS)

Journal: Journal of the American Chemical Society

Quartile SCImago

Quartile WOS

Impact factor: 15

ISSN: 00027863, 15205126

DOI: 10.1021/jacs.9b08357

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General Chemistry

Catalysis

Biochemistry

Colloid and Surface Chemistry

Abstract

We report on a new family of argyrodite lithium superionic conductors, as solid solutions Li6+xMxSb1-xS5I (M = Si, Ge, Sn), that exhibit superionic conductivity. These represent the first antimony argyrodites to date. Exploration of the series using a combination of single crystal X-ray and synchrotron/neutron powder diffraction, combined with impedance spectroscopy, reveals that an optimal degree of substitution (x), and substituent induces slight S2-/I- anion site disorder-but more importantly drives Li+ cation site disorder. The additional, delocalized Li-ion density is located in new high energy lattice sites that provide intermediate interstitial positions (local minima) for Li+ diffusion and activate concerted ion migration, leading to a low activation energy of 0.25 eV. Excellent room temperature ionic conductivity of 14.8 mS·cm-1 is exhibited for cold-pressed pellets-up to 24 mS·cm-1 for sintered pellets-among the highest values reported to date. This enables all-solid-state battery prototypes that exhibit promising properties. Furthermore, even at -78 °C, suitable bulk ionic conductivity of the electrolyte is retained (0.25 mS·cm-1). Selected thioantimonate iodides demonstrate good compatibility with Li metal, sustaining over 1000 h of Li stripping/plating at current densities up to 0.6 mA·cm-2. The significantly enhanced Li ion conduction and lowered activation energy barrier with increasing site disorder reveals an important strategy toward the development of superionic conductors.

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Citations by journals

	2 4 6 8 10 12 14 16 18 20
Chemistry of Materials	Chemistry of Materials, 19, 7.36% Chemistry of Materials 19 publications, 7.36%
Advanced Energy Materials	Advanced Energy Materials, 17, 6.59% Advanced Energy Materials 17 publications, 6.59%
ACS Energy Letters	ACS Energy Letters, 9, 3.49% ACS Energy Letters 9 publications, 3.49%
Journal of the American Chemical Society	Journal of the American Chemical Society, 8, 3.1% Journal of the American Chemical Society 8 publications, 3.1%
Energy Storage Materials	Energy Storage Materials, 7, 2.71% Energy Storage Materials 7 publications, 2.71%
Angewandte Chemie - International Edition	Angewandte Chemie - International Edition, 7, 2.71% Angewandte Chemie - International Edition 7 publications, 2.71%
Angewandte Chemie	Angewandte Chemie, 7, 2.71% Angewandte Chemie 7 publications, 2.71%
Advanced Functional Materials	Advanced Functional Materials, 7, 2.71% Advanced Functional Materials 7 publications, 2.71%
Journal of Materials Chemistry A	Journal of Materials Chemistry A, 7, 2.71% Journal of Materials Chemistry A 7 publications, 2.71%
ACS Applied Energy Materials	ACS Applied Energy Materials, 6, 2.33% ACS Applied Energy Materials 6 publications, 2.33%
ACS applied materials & interfaces	ACS applied materials & interfaces, 6, 2.33% ACS applied materials & interfaces 6 publications, 2.33%
Journal of Power Sources	Journal of Power Sources, 5, 1.94% Journal of Power Sources 5 publications, 1.94%
Energy and Environmental Science	Energy and Environmental Science, 5, 1.94% Energy and Environmental Science 5 publications, 1.94%
Materials Advances	Materials Advances, 5, 1.94% Materials Advances 5 publications, 1.94%
Nature Communications	Nature Communications, 4, 1.55% Nature Communications 4 publications, 1.55%
Advanced Science	Advanced Science, 4, 1.55% Advanced Science 4 publications, 1.55%
Batteries & Supercaps	Batteries & Supercaps, 4, 1.55% Batteries & Supercaps 4 publications, 1.55%
Inorganic Chemistry	Inorganic Chemistry, 4, 1.55% Inorganic Chemistry 4 publications, 1.55%
ACS Materials Letters	ACS Materials Letters, 3, 1.16% ACS Materials Letters 3 publications, 1.16%
Applied Physics Letters	Applied Physics Letters, 3, 1.16% Applied Physics Letters 3 publications, 1.16%
Nature Energy	Nature Energy, 3, 1.16% Nature Energy 3 publications, 1.16%
Electrochemical Energy Reviews	Electrochemical Energy Reviews, 3, 1.16% Electrochemical Energy Reviews 3 publications, 1.16%
Journal of Energy Chemistry	Journal of Energy Chemistry, 3, 1.16% Journal of Energy Chemistry 3 publications, 1.16%
Chemical Engineering Journal	Chemical Engineering Journal, 3, 1.16% Chemical Engineering Journal 3 publications, 1.16%
Solid State Ionics	Solid State Ionics, 3, 1.16% Solid State Ionics 3 publications, 1.16%
Small Methods	Small Methods, 3, 1.16% Small Methods 3 publications, 1.16%
Nano Energy	Nano Energy, 3, 1.16% Nano Energy 3 publications, 1.16%
Energy Technology	Energy Technology, 3, 1.16% Energy Technology 3 publications, 1.16%
Advanced Materials	Advanced Materials, 3, 1.16% Advanced Materials 3 publications, 1.16%
	2 4 6 8 10 12 14 16 18 20

Citations by publishers

	10 20 30 40 50 60 70 80
Wiley	Wiley, 71, 27.52% Wiley 71 publications, 27.52%
American Chemical Society (ACS)	American Chemical Society (ACS), 65, 25.19% American Chemical Society (ACS) 65 publications, 25.19%
Elsevier	Elsevier, 43, 16.67% Elsevier 43 publications, 16.67%
Royal Society of Chemistry (RSC)	Royal Society of Chemistry (RSC), 25, 9.69% Royal Society of Chemistry (RSC) 25 publications, 9.69%
Springer Nature	Springer Nature, 21, 8.14% Springer Nature 21 publications, 8.14%
IOP Publishing	IOP Publishing, 4, 1.55% IOP Publishing 4 publications, 1.55%
American Institute of Physics (AIP)	American Institute of Physics (AIP), 3, 1.16% American Institute of Physics (AIP) 3 publications, 1.16%
International Union of Crystallography (IUCr)	International Union of Crystallography (IUCr), 2, 0.78% International Union of Crystallography (IUCr) 2 publications, 0.78%
National Academy of Sciences of Ukraine - Institute of Semiconductor Physics	National Academy of Sciences of Ukraine - Institute of Semiconductor Physics, 2, 0.78% National Academy of Sciences of Ukraine - Institute of Semiconductor Physics 2 publications, 0.78%
Chinese Physical Society	Chinese Physical Society, 2, 0.78% Chinese Physical Society 2 publications, 0.78%
Multidisciplinary Digital Publishing Institute (MDPI)	Multidisciplinary Digital Publishing Institute (MDPI), 2, 0.78% Multidisciplinary Digital Publishing Institute (MDPI) 2 publications, 0.78%
American Association for the Advancement of Science (AAAS)	American Association for the Advancement of Science (AAAS), 2, 0.78% American Association for the Advancement of Science (AAAS) 2 publications, 0.78%
Research Square Platform LLC	Research Square Platform LLC, 2, 0.78% Research Square Platform LLC 2 publications, 0.78%
The Royal Society	The Royal Society, 1, 0.39% The Royal Society 1 publication, 0.39%
The Electrochemical Society	The Electrochemical Society, 1, 0.39% The Electrochemical Society 1 publication, 0.39%
Japan Institute of Metals and Materials	Japan Institute of Metals and Materials, 1, 0.39% Japan Institute of Metals and Materials 1 publication, 0.39%
Frontiers Media S.A.	Frontiers Media S.A., 1, 0.39% Frontiers Media S.A. 1 publication, 0.39%
Taylor & Francis	Taylor & Francis, 1, 0.39% Taylor & Francis 1 publication, 0.39%
Institute of Physical Optics	Institute of Physical Optics, 1, 0.39% Institute of Physical Optics 1 publication, 0.39%
Naukova Dumka	Naukova Dumka, 1, 0.39% Naukova Dumka 1 publication, 0.39%
Hans Publishers	Hans Publishers, 1, 0.39% Hans Publishers 1 publication, 0.39%
OAE Publishing Inc.	OAE Publishing Inc., 1, 0.39% OAE Publishing Inc. 1 publication, 0.39%
Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii	Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii, 1, 0.39% Autonomous Non-profit Organization Editorial Board of the journal Uspekhi Khimii 1 publication, 0.39%
	10 20 30 40 50 60 70 80

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Zhou L. et al. New Family of Argyrodite Thioantimonate Lithium Superionic Conductors // Journal of the American Chemical Society. 2019. Vol. 141. No. 48. pp. 19002-19013.

GOST all authors (up to 50) Copy

Zhou L., Assoud A., Singh V. K., Wu X., Nazar L. F. New Family of Argyrodite Thioantimonate Lithium Superionic Conductors // Journal of the American Chemical Society. 2019. Vol. 141. No. 48. pp. 19002-19013.

RIS |

Cite this

RIS Copy

TY - JOUR

DO - 10.1021/jacs.9b08357

UR - https://doi.org/10.1021/jacs.9b08357

TI - New Family of Argyrodite Thioantimonate Lithium Superionic Conductors

T2 - Journal of the American Chemical Society

AU - Wu, Xiaohan

AU - Zhou, Laidong

AU - Nazar, Linda F.

AU - Assoud, Abdeljalil

AU - Singh, Vijay Kumar

PY - 2019

DA - 2019/10/23 00:00:00

PB - American Chemical Society (ACS)

SP - 19002-19013

IS - 48

VL - 141

SN - 0002-7863

SN - 1520-5126

ER -

BibTex |

Cite this

BibTex Copy

@article{2019_Zhou,

author = {Xiaohan Wu and Laidong Zhou and Linda F. Nazar and Abdeljalil Assoud and Vijay Kumar Singh},

title = {New Family of Argyrodite Thioantimonate Lithium Superionic Conductors},

journal = {Journal of the American Chemical Society},

year = {2019},

volume = {141},

publisher = {American Chemical Society (ACS)},

month = {oct},

url = {https://doi.org/10.1021/jacs.9b08357},

number = {48},

pages = {19002--19013},

doi = {10.1021/jacs.9b08357}

}

MLA

Cite this

MLA Copy

Zhou, Laidong, et al. “New Family of Argyrodite Thioantimonate Lithium Superionic Conductors.” Journal of the American Chemical Society, vol. 141, no. 48, Oct. 2019, pp. 19002-19013. https://doi.org/10.1021/jacs.9b08357.

Found error?

Publisher

American Chemical Society (ACS)

Journal

Journal of the American Chemical Society

Quartile SCImago

Quartile WOS

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ISSN

00027863 (Print)
15205126 (Electronic)