Molecular Dynamics Modeling of the Structure and Na+-Ion Transport in Na2S + SiS2 Glassy Electrolytes

Dive, A.; Benmore, C.; Wilding, M.; Martin, S. W.; Beckman, S.; Banerjee, Soumik

doi:10.1021/acs.jpcb.8b04353

Title: Molecular Dynamics Modeling of the Structure and Na⁺-Ion Transport in Na₂S + SiS₂ Glassy Electrolytes

Abstract

Solid-state sodium batteries, a relatively safe and potentially cost-effective energy-storage technology, have attracted increasing scientific attention recently for application in stationary grid-scale energy storage. Identifying solid electrolytes with high electrochemical stability and high Na+-ion conductivity at room temperature is critically important to enable high energy densities with enhanced rate capabilities. We evaluated sodium sulfide silicon sulfide, xNa₂S + (1 - x)SiS₂, glasses as potential glassy solid electrolytes (GSEs) using molecular dynamics (MD) simulations. We employed ab initio MD to determine ion conduction mechanisms, to calculate energy barriers for ion hops, and to correlate these to the local short-range structure of 0.50Na₂S + 0.50SiS₂ glass. To simulate much larger systems for accurately calculating the ionic conductivity, we parameterized empirical Buckingham-type potential and performed classical MD simulations. After validating these calculations by comparing the structure obtained from MD to that from X-ray scattering data, we calculated the ionic conductivity of these glasses for the range of 0.33 ≤ x ≤ 0.67 compositions. The calculated ionic conductivities at room temperature were in the range of similar to 10^-5 S/cm for the x = 0.50 composition and increased significantly with sodium sulfide (x) content. Furthermore, these calculations provide theoretical insights into the role ofmore »« less

Authors:

^[1]; Benmore, C. ^[2]; Wilding, M. ^[3]; Martin, S. W. ^[4]; Beckman, S. ^[1];

^[1]

Washington State Univ., Pullman, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. College London, London (United Kingdom)
Iowa State Univ., Ames, IA (United States)

Publication Date:: Wed Jun 20 00:00:00 EDT 2018

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Advanced Research Projects Agency - Energy (ARPA-E)

OSTI Identifier:: 1480490

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

Additional Journal Information:: Journal Volume: 122; Journal Issue: 30; Journal ID: ISSN 1520-6106

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE; Na ion battery; ionic conductivity; molecular dynamics; sodium sulfide glass

Citation Formats


                    Dive, A., Benmore, C., Wilding, M., Martin, S. W., Beckman, S., and Banerjee, Soumik. Molecular Dynamics Modeling of the Structure and Na+-Ion Transport in Na2S + SiS2 Glassy Electrolytes.  United States: N. p., 2018. 
Web.  doi:10.1021/acs.jpcb.8b04353.

Copy to clipboard


                    Dive, A., Benmore, C., Wilding, M., Martin, S. W., Beckman, S., & Banerjee, Soumik. Molecular Dynamics Modeling of the Structure and Na+-Ion Transport in Na2S + SiS2 Glassy Electrolytes.  United States.  https://doi.org/10.1021/acs.jpcb.8b04353

Copy to clipboard


                    Dive, A., Benmore, C., Wilding, M., Martin, S. W., Beckman, S., and Banerjee, Soumik. Wed .  
"Molecular Dynamics Modeling of the Structure and Na+-Ion Transport in Na2S + SiS2 Glassy Electrolytes".  United States.  https://doi.org/10.1021/acs.jpcb.8b04353.  https://www.osti.gov/servlets/purl/1480490.

Copy to clipboard


                    
@article{osti_1480490,

  title        = {Molecular Dynamics Modeling of the Structure and Na+-Ion Transport in Na2S + SiS2 Glassy Electrolytes},

  author       = {Dive, A. and Benmore, C. and Wilding, M. and Martin, S. W. and Beckman, S. and Banerjee, Soumik},

  abstractNote = {Solid-state sodium batteries, a relatively safe and potentially cost-effective energy-storage technology, have attracted increasing scientific attention recently for application in stationary grid-scale energy storage. Identifying solid electrolytes with high electrochemical stability and high Na+-ion conductivity at room temperature is critically important to enable high energy densities with enhanced rate capabilities. We evaluated sodium sulfide silicon sulfide, xNa2S + (1 - x)SiS2, glasses as potential glassy solid electrolytes (GSEs) using molecular dynamics (MD) simulations. We employed ab initio MD to determine ion conduction mechanisms, to calculate energy barriers for ion hops, and to correlate these to the local short-range structure of 0.50Na2S + 0.50SiS2 glass. To simulate much larger systems for accurately calculating the ionic conductivity, we parameterized empirical Buckingham-type potential and performed classical MD simulations. After validating these calculations by comparing the structure obtained from MD to that from X-ray scattering data, we calculated the ionic conductivity of these glasses for the range of 0.33 ≤ x ≤ 0.67 compositions. The calculated ionic conductivities at room temperature were in the range of similar to 10-5 S/cm for the x = 0.50 composition and increased significantly with sodium sulfide (x) content. Furthermore, these calculations provide theoretical insights into the role of Na2S content on the ionic conductivity of GSEs aiding in the selection of specific compositions to enhance the ionic conductivity.},

  doi          = {10.1021/acs.jpcb.8b04353},

  journal      = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},

  number       = 30,

  volume       = 122,

  place        = {United States},

  year         = {Wed Jun 20 00:00:00 EDT 2018},

  month        = {Wed Jun 20 00:00:00 EDT 2018}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1021/acs.jpcb.8b04353

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 12 works

Citation information provided by
Web of Science

Figures / Tables:

Table 1: Basis sets and pseudopotentials utilized for ab initio MD simulations are reported.

All figures and tables (17 total)

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Electrical Energy Storage for the Grid: A Battery of Choices
journal, November 2011

Dunn, B.; Kamath, H.; Tarascon, J. -M.
Science, Vol. 334, Issue 6058
DOI: 10.1126/science.1212741

Basic Research Needs for Electrical Energy Storage. Report of the Basic Energy Sciences Workshop on Electrical Energy Storage, April 2-4, 2007
report, April 2007

Goodenough, J. B.; Abruna, H. D.; Buchanan, M. V.
DOI: 10.2172/935429

Advances and challenges of sodium ion batteries as post lithium ion batteries
journal, January 2015

Sawicki, Monica; Shaw, Leon L.
RSC Advances, Vol. 5, Issue 65
DOI: 10.1039/C5RA08321D

Current trends and future challenges of electrolytes for sodium-ion batteries
journal, January 2016

Vignarooban, K.; Kushagra, R.; Elango, A.
International Journal of Hydrogen Energy, Vol. 41, Issue 4
DOI: 10.1016/j.ijhydene.2015.12.090

Main Challenges for High Performance NAS Battery: Materials and Interfaces
journal, May 2012

Wen, Zhaoyin; Hu, Yingying; Wu, Xiangwei
Advanced Functional Materials, Vol. 23, Issue 8
DOI: 10.1002/adfm.201200473

Research Development on Sodium-Ion Batteries
journal, October 2014

Yabuuchi, Naoaki; Kubota, Kei; Dahbi, Mouad
Chemical Reviews, Vol. 114, Issue 23
DOI: 10.1021/cr500192f

Sodium and sodium-ion energy storage batteries
journal, August 2012

Ellis, Brian L.; Nazar, Linda F.
Current Opinion in Solid State and Materials Science, Vol. 16, Issue 4, p. 168-177
DOI: 10.1016/j.cossms.2012.04.002

Parametric study of dry coating process of electrode particle with model material of sulfide solid electrolytes for all-solid-state battery
journal, January 2017

Kawaguchi, Takashi; Nakamura, Hideya; Watano, Satoru
Powder Technology, Vol. 305
DOI: 10.1016/j.powtec.2016.09.085

Room-temperature stationary sodium-ion batteries for large-scale electric energy storage
journal, January 2013

Pan, Huilin; Hu, Yong-Sheng; Chen, Liquan
Energy & Environmental Science, Vol. 6, Issue 8
DOI: 10.1039/c3ee40847g

Sodium-ion batteries: present and future
journal, January 2017

Hwang, Jang-Yeon; Myung, Seung-Taek; Sun, Yang-Kook
Chemical Society Reviews, Vol. 46, Issue 12
DOI: 10.1039/C6CS00776G

Superionic glass-ceramic electrolytes for room-temperature rechargeable sodium batteries
journal, January 2012

Hayashi, Akitoshi; Noi, Kousuke; Sakuda, Atsushi
Nature Communications, Vol. 3, Issue 1
DOI: 10.1038/ncomms1843

Sulfide Glass-Ceramic Electrolytes for All-Solid-State Lithium and Sodium Batteries
journal, July 2014

Tatsumisago, Masahiro; Hayashi, Akitoshi
International Journal of Applied Glass Science, Vol. 5, Issue 3
DOI: 10.1111/ijag.12084

Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na ₃ PSe ₄
journal, December 2015

Bo, Shou-Hang; Wang, Yan; Kim, Jae Chul
Chemistry of Materials, Vol. 28, Issue 1
DOI: 10.1021/acs.chemmater.5b04013

Na ₃ PSe ₄ : A Novel Chalcogenide Solid Electrolyte with High Ionic Conductivity
journal, October 2015

Zhang, Long; Yang, Kun; Mi, Jianli
Advanced Energy Materials, Vol. 5, Issue 24
DOI: 10.1002/aenm.201501294

An Air-Stable Na ₃ SbS ₄ Superionic Conductor Prepared by a Rapid and Economic Synthetic Procedure
journal, June 2016

Wang, Hui; Chen, Yan; Hood, Zachary D.
Angewandte Chemie International Edition, Vol. 55, Issue 30
DOI: 10.1002/anie.201601546

Design and synthesis of the superionic conductor Na10SnP2S12
journal, March 2016

Richards, William D.; Tsujimura, Tomoyuki; Miara, Lincoln J.
Nature Communications, Vol. 7, Issue 1
DOI: 10.1038/ncomms11009

Fast ion motion in glassy and amorphous materials
journal, December 1983

Angell, C.
Solid State Ionics, Vol. 9-10
DOI: 10.1016/0167-2738(83)90206-0

Fast ion conducting glasses
journal, August 1985

Minami, Tsutomu
Journal of Non-Crystalline Solids, Vol. 73, Issue 1-3
DOI: 10.1016/0022-3093(85)90353-9

Transport studies on mechanochemically synthesized amorphous AgI–Ag2 O–CrO3 superionic system
journal, April 2003

Dalvi, A.
Solid State Ionics, Vol. 159, Issue 3-4
DOI: 10.1016/S0167-2738(03)00003-1

Phase transition and the ${Ag}^{+}$ -ion diffusion in AgI: Effect of homovalent ${Br}^{-}$ -ion substitution
journal, June 1981

Shahi, K.; Wagner, J. B.
Physical Review B, Vol. 23, Issue 12
DOI: 10.1103/PhysRevB.23.6417

Ionic conductivity of glasses in the MI+M2S+(0.1Ga2S3+0.9GeS2) system (M=Li, Na, K and Cs)
journal, January 2008

Yao, W.; Martin, S.
Solid State Ionics, Vol. 178, Issue 33-34
DOI: 10.1016/j.ssi.2007.10.011

Development of Sulfide Solid Electrolytes and Interface Formation Processes for Bulk-Type All-Solid-State Li and Na Batteries
journal, July 2016

Hayashi, Akitoshi; Sakuda, Atsushi; Tatsumisago, Masahiro
Frontiers in Energy Research, Vol. 4
DOI: 10.3389/fenrg.2016.00025

Recent progress of glass and glass-ceramics as solid electrolytes for lithium secondary batteries
journal, October 2006

Minami, T.; Hayashi, A.; Tatsumisago, M.
Solid State Ionics, Vol. 177, Issue 26-32
DOI: 10.1016/j.ssi.2006.07.017

Structural investigations of yNa2S+(1−y)PS5/2 glasses using Raman and infrared spectroscopies
journal, December 2012

Bischoff, Christian; Schuller, Katherine; Haynes, Michael
Journal of Non-Crystalline Solids, Vol. 358, Issue 23
DOI: 10.1016/j.jnoncrysol.2012.09.023

Preparation and characterization of highly sodium ion conducting Na ₃ PS ₄ –Na ₄ SiS ₄ solid electrolytes
journal, January 2014

Tanibata, Naoto; Noi, Kousuke; Hayashi, Akitoshi
RSC Adv., Vol. 4, Issue 33
DOI: 10.1039/C4RA00996G

High lithium ion conducting glass-ceramics in the system Li2S–P2S5
journal, October 2006

Mizuno, F.; Hayashi, A.; Tadanaga, K.
Solid State Ionics, Vol. 177, Issue 26-32
DOI: 10.1016/j.ssi.2006.04.017

A sulphide lithium super ion conductor is superior to liquid ion conductors for use in rechargeable batteries
journal, January 2014

Seino, Yoshikatsu; Ota, Tsuyoshi; Takada, Kazunori
Energy Environ. Sci., Vol. 7, Issue 2
DOI: 10.1039/C3EE41655K

Calculation of Activation Energy of Ionic Conductivity in Silica Glasses by Classical Methods
journal, December 1954

Anderson, O. L.; Stuart, D. A.
Journal of the American Ceramic Society, Vol. 37, Issue 12
DOI: 10.1111/j.1151-2916.1954.tb13991.x

Glasses as solid electrolytes
journal, May 1980

Ravaine, D.
Journal of Non-Crystalline Solids, Vol. 38-39
DOI: 10.1016/0022-3093(80)90444-5

Ionic Conductivity of Mixed Glass Former 0.35Na ₂ O + 0.65[ x B ₂ O ₃ + (1 – x )P ₂ O ₅ ] Glasses
journal, December 2013

Christensen, Randilynn; Olson, Garrett; Martin, Steve W.
The Journal of Physical Chemistry B, Vol. 117, Issue 51
DOI: 10.1021/jp409497z

Activation Enthalpy for Diffusion in Glass
journal, October 1986

McElfresh, DavidK.; Howitt, Dvid G.
Journal of the American Ceramic Society, Vol. 69, Issue 10
DOI: 10.1111/j.1151-2916.1986.tb07347.x

Lithium and sodium battery cathode materials: computational insights into voltage, diffusion and nanostructural properties
journal, January 2014

Islam, M. Saiful; Fisher, Craig A. J.
Chem. Soc. Rev., Vol. 43, Issue 1
DOI: 10.1039/C3CS60199D

Sodium Ion Diffusion and Voltage Trends in Phosphates Na ₄ M ₃ (PO ₄ ) ₂ P ₂ O ₇ (M = Fe, Mn, Co, Ni) for Possible High-Rate Cathodes
journal, June 2015

Wood, Stephen M.; Eames, Chris; Kendrick, Emma
The Journal of Physical Chemistry C, Vol. 119, Issue 28
DOI: 10.1021/acs.jpcc.5b04648

Design of Li _1+2x Zn _1−x PS ₄ , a new lithium ion conductor
journal, January 2016

Richards, William D.; Wang, Yan; Miara, Lincoln J.
Energy & Environmental Science, Vol. 9, Issue 10
DOI: 10.1039/C6EE02094A

Structural and Na-ion conduction characteristics of Na ₃ PS _x Se _4−x
journal, January 2016

Bo, Shou-Hang; Wang, Yan; Ceder, Gerbrand
Journal of Materials Chemistry A, Vol. 4, Issue 23
DOI: 10.1039/C6TA03027K

Interface Stability in Solid-State Batteries
journal, December 2015

Richards, William D.; Miara, Lincoln J.; Wang, Yan
Chemistry of Materials, Vol. 28, Issue 1
DOI: 10.1021/acs.chemmater.5b04082

State of the Art and Future Research Needs for Multiscale Analysis of Li-Ion Cells
journal, May 2017

Shah, K.; Balsara, N.; Banerjee, S.
Journal of Electrochemical Energy Conversion and Storage, Vol. 14, Issue 2
DOI: 10.1115/1.4036456

Molecular Dynamics Simulation of the Effect of Crystal Orientation on Lithium‐Ion Diffusion at the V 2 O 5 / Li2SiO3 Interface
journal, March 1999

Garcia, M. E.; Garofalini, S. H.
Journal of The Electrochemical Society, Vol. 146, Issue 3
DOI: 10.1149/1.1391690

Lithium Ion Diffusion Mechanism in Lithium Lanthanum Titanate Solid-State Electrolytes from Atomistic Simulations
journal, November 2014

Chen, Chao-hsu; Du, Jincheng
Journal of the American Ceramic Society, Vol. 98, Issue 2
DOI: 10.1111/jace.13307

High power lithium ion battery materials by computational design
journal, July 2011

Adams, Stefan; Rao, R. Prasada
physica status solidi (a), Vol. 208, Issue 8
DOI: 10.1002/pssa.201001116

A combined molecular dynamics simulation, experimental and coupling model study of the ion dynamics in glassy ionic conductors
journal, April 2003

Ngai, K. L.; Habasaki, J.; Hiwatari, Y.
Journal of Physics: Condensed Matter, Vol. 15, Issue 16
DOI: 10.1088/0953-8984/15/16/310

Molecular dynamics simulations of structural changes in mixed alkali (Li–K) silicate glasses
journal, September 1999

Park, Byeongwon; Cormack, A. N.
Journal of Non-Crystalline Solids, Vol. 255, Issue 1
DOI: 10.1016/S0022-3093(99)00430-5

A new interpretation of the dynamic structure model of ion transport in molten and solid glasses
journal, January 2004

Bunde, Armin; Ingram, Malcolm D.; Russ, Stefanie
Phys. Chem. Chem. Phys., Vol. 6, Issue 13
DOI: 10.1039/B316738K

Complete Identification of Alkali Sites in Ion Conducting Lithium Silicate Glasses: A Computer Study of Ion Dynamics
journal, May 2003

Lammert, Heiko; Kunow, Magnus; Heuer, Andreas
Physical Review Letters, Vol. 90, Issue 21
DOI: 10.1103/PhysRevLett.90.215901

Quickstep: Fast and accurate density functional calculations using a mixed Gaussian and plane waves approach
journal, April 2005

VandeVondele, Joost; Krack, Matthias; Mohamed, Fawzi
Computer Physics Communications, Vol. 167, Issue 2
DOI: 10.1016/j.cpc.2004.12.014

cp2k: atomistic simulations of condensed matter systems
journal, June 2013

Hutter, Jürg; Iannuzzi, Marcella; Schiffmann, Florian
Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 4, Issue 1
DOI: 10.1002/wcms.1159

Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases
journal, September 2007

VandeVondele, Joost; Hutter, Jürg
The Journal of Chemical Physics, Vol. 127, Issue 11
DOI: 10.1063/1.2770708

Molecular dynamics studies of the vitreous state: Simple ionic systems and silica
journal, August 1976

Woodcock, L. V.; Angell, C. A.; Cheeseman, P.
The Journal of Chemical Physics, Vol. 65, Issue 4
DOI: 10.1063/1.433213

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
DOI: 10.1063/1.1329672

Nudged-elastic band method with two climbing images: Finding transition states in complex energy landscapes
journal, January 2015

Zarkevich, Nikolai A.; Johnson, Duane D.
The Journal of Chemical Physics, Vol. 142, Issue 2
DOI: 10.1063/1.4905209

Optimization methods for finding minimum energy paths
journal, April 2008

Sheppard, Daniel; Terrell, Rye; Henkelman, Graeme
The Journal of Chemical Physics, Vol. 128, Issue 13
DOI: 10.1063/1.2841941

The classical equation of state of gaseous helium, neon and argon
journal, October 1938

Buckingham, R. A.
Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 168, Issue 933, p. 264-283
DOI: 10.1098/rspa.1938.0173

New interatomic potential parameters for molecular dynamics simulations of rare-earth (RE = La, Y, Lu, Sc) aluminosilicate glass structures: exploration of RE3+ field-strength effects
journal, January 2013

Okhotnikov, Kirill; Stevensson, Baltzar; Edén, Mattias
Physical Chemistry Chemical Physics, Vol. 15, Issue 36
DOI: 10.1039/c3cp51726h

A New Self-Consistent Empirical Interatomic Potential Model for Oxides, Silicates, and Silica-Based Glasses
journal, June 2006

Pedone, Alfonso; Malavasi, Gianluca; Menziani, M. Cristina
The Journal of Physical Chemistry B, Vol. 110, Issue 24
DOI: 10.1021/jp0611018

Shell-model molecular dynamics calculations of modified silicate glasses
journal, March 2006

Tilocca, Antonio; de Leeuw, Nora H.; Cormack, Alastair N.
Physical Review B, Vol. 73, Issue 10
DOI: 10.1103/PhysRevB.73.104209

Molecular dynamics study of Li2SiS3 glass
journal, October 1996

Seshasayee, M.
Solid State Ionics, Vol. 91, Issue 3-4
DOI: 10.1016/S0167-2738(96)00449-3

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Plimpton, Steve
Journal of Computational Physics, Vol. 117, Issue 1
DOI: 10.1006/jcph.1995.1039

Li ⁺ Cation Environment, Transport, and Mechanical Properties of the LiTFSI Doped N -Methyl- N -alkylpyrrolidinium ⁺ TFSI ^- Ionic Liquids
journal, August 2006

Borodin, Oleg; Smith, Grant D.; Henderson, Wesley
The Journal of Physical Chemistry B, Vol. 110, Issue 34
DOI: 10.1021/jp061930t

Area detector corrections for high quality synchrotron X-ray structure factor measurements
journal, January 2012

Skinner, Lawrie B.; Benmore, Chris J.; Parise, John B.
Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 662, Issue 1
DOI: 10.1016/j.nima.2011.09.031

Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996

Hammersley, A. P.; Svensson, S. O.; Hanfland, M.
High Pressure Research, Vol. 14, Issue 4-6, p. 235-248
DOI: 10.1080/08957959608201408

PDFgetX2: a GUI-driven program to obtain the pair distribution function from X-ray powder diffraction data
journal, July 2004

Qiu, Xiangyun; Thompson, Jeroen W.; Billinge, Simon J. L.
Journal of Applied Crystallography, Vol. 37, Issue 4, p. 678-678
DOI: 10.1107/S0021889804011744

Short range order characterization of the Na2S + SiS2 glass system using Raman, infrared and 29Si magic angle spinning nuclear magnetic resonance spectroscopies
journal, September 2017

Watson, Deborah E.; Martin, Steve W.
Journal of Non-Crystalline Solids, Vol. 471
DOI: 10.1016/j.jnoncrysol.2017.04.032

Lattice dynamics of Na ₂ S
journal, October 1980

Buhrer, W.; Bill, H.
Journal of Physics C: Solid State Physics, Vol. 13, Issue 30
DOI: 10.1088/0022-3719/13/30/014

Works referencing / citing this record:

Recent Research on Strategies to Improve Ion Conduction in Alkali Metal‐Ion Batteries
journal, April 2019

Shao, TieLei; Liu, Chunyi; Deng, Wenjun
Batteries & Supercaps, Vol. 2, Issue 5
DOI: 10.1002/batt.201800147

Figures / Tables found in this record:

Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

Similar Records in DOE PAGES and OSTI.GOV collections:

Structures and ionic conduction of xNa{sub 2}S + (1-x)SiS{sub 2} glasses

Conference Cho, J ; Martin, S W

Studies of the structures and the compositionally dependent conductivity of xNa{sub 2}S + (1-x)SiS{sub 2} glasses have been carried out for the first time. Infrared spectroscopy has been chosen as the structure sensitive probe because it is sensitive to short range order (SRO) in glass and crystals. The IR spectra of the sodium metathiosilicate (x = 0.5) and orthothiosilicate (x = 0.66) polycrystals indicate that the increasing amounts of Na{sub 2}S give rise to the formation of ionic SiS{sub 4}{sup 4-} groups, which result from severing covalent Si-S-Si linkages. Likewise, the IR spectra of the sodium thiosilicate glasses indicates themore »« less
Origin of Outstanding Phase and Moisture Stability in a Na₃P_1–x As_xS₄ Superionic Conductor

Journal Article Shang, Shun-Li ; Yu, Zhaoxin ; Wang, Yi ; ... - ACS Applied Materials and Interfaces

Sodium ion (Na) solid-state electrolytes (SSEs) are critical to address notorious safety issues associated with liquid electrolytes used in the current Na ion batteries. Fulfilling multiple innovations is a grand challenge but is imperative for advanced Na ion SSEs, such as a combination of high ionic conductivity and excellent chemical stability. Here, our first-principles and phonon calculations reveal that Na₃P_1–xAs_xS₄ (0 ≤ x ≤ 1) is a solid-state superionic conductor stabilized at 0 K by zero-point vibrational energy and at finite temperatures by vibrational and configurational entropies. Especially, our integrated first-principles and experimental approach indicates that Na₃P_1–xAs_xS₄ is dry-air stable. Additionally, the alloying element arsenic greatly enhances the moisture (i.e., H₂O) stability of Na₃P_1–xAs_xS₄ by shifting the reaction products from the easy-forming oxysulfides (such as Na₃POS₃ and Na₃PO₂S₂ with H₂S release) to the difficult-forming hydrates (such as Na₃P_1–xAs_xS₄·more »« less
Cited by 40
https://doi.org/10.1021/acsami.7b03606

Full Text Available
Ionic Conduction in Cubic Na ₃ TiP ₃ O ₉ N, a Secondary Na-Ion Battery Cathode with Extremely Low Volume Change

Journal Article Liu, Jue ; Chang, Donghee ; Whitfield, Pamela ; ... - Chemistry of Materials

We demonstrate that Na ions are mobile at room temperature in the nitridophosphate compound Na₃TiP₃O₉N, with a diffusion pathway that is calculated to be fully three-dimensional and isotropic. When used as a cathode in Na-ion batteries, Na₃TiP₃O₉N has an average voltage of 2.7 V vs Na⁺/Na and cycles with good reversibility through a mechanism that appears to be a single solid solution process without any intermediate plateaus. X-ray and neutron diffraction studies as well as first-principles calculations indicate that the volume change that occurs on Na-ion removal is only about 0.5%, a remarkably small volume change given the large ionicmore »« less
https://doi.org/10.1021/cm5011218
Studies of Functional Defects for Fast Na-Ion Conduction in Na _3-_yPS_4-_xCl_x with a Combined Experimental and Computational Approach

Journal Article Feng, Xuyong ; Chien, Po-Hsiu ; Zhu, Zhuoying ; ... - Advanced Functional Materials

Abstract All‐solid‐state rechargeable sodium (Na)‐ion batteries are promising for inexpensive and high‐energy‐density large‐scale energy storage. In this contribution, new Na solid electrolytes, Na ₃₋ _y PS ₄₋ _x Cl _x , are synthesized with a strategic approach, which allows maximum substitution of Cl for S ( x = 0.2) without significant compromise of structural integrity or Na deficiency. A maximum conductivity of 1.96 mS cm ⁻¹ at 25 °C is achieved for Na _3.0 PS _3.8 Cl _0.2 , which is two orders of magnitude higher compared with that of tetragonal Na ₃ PS ₄ (t‐Na ₃ PS ₄ ).more »« less
Cited by 34
https://doi.org/10.1002/adfm.201807951

Full Text Available
Design and synthesis of the superionic conductor Na₁₀SnP₂S₁₂

Journal Article Richards, William D. ; Tsujimura, Tomoyuki ; Miara, Lincoln J. ; ... - Nature Communications

Sodium-ion batteries are emerging as candidates for large-scale energy storage due to their low cost and the wide variety of cathode materials available. As battery size and adoption in critical applications increases, safety concerns are resurfacing due to the inherent flammability of organic electrolytes currently in use in both lithium and sodium battery chemistries. Development of solid-state batteries with ionic electrolytes eliminates this concern, while also allowing novel device architectures and potentially improving cycle life. Here we report the computation-assisted discovery and synthesis of a high-performance solid-state electrolyte material: Na₁₀SnP₂S₁₂, with room temperature ionic conductivity of 0.4 mS cm^-1 rivallingmore »« less
Cited by 217
https://doi.org/10.1038/ncomms11009

Full Text Available

Similar Records

Title: Molecular Dynamics Modeling of the Structure and Na+-Ion Transport in Na2S + SiS2 Glassy Electrolytes

Abstract

Citation Formats

Figures / Tables:

Electrical Energy Storage for the Grid: A Battery of Choices journal, November 2011

Basic Research Needs for Electrical Energy Storage. Report of the Basic Energy Sciences Workshop on Electrical Energy Storage, April 2-4, 2007 report, April 2007

Advances and challenges of sodium ion batteries as post lithium ion batteries journal, January 2015

Current trends and future challenges of electrolytes for sodium-ion batteries journal, January 2016

Main Challenges for High Performance NAS Battery: Materials and Interfaces journal, May 2012

Research Development on Sodium-Ion Batteries journal, October 2014

Sodium and sodium-ion energy storage batteries journal, August 2012

Parametric study of dry coating process of electrode particle with model material of sulfide solid electrolytes for all-solid-state battery journal, January 2017

Room-temperature stationary sodium-ion batteries for large-scale electric energy storage journal, January 2013

Sodium-ion batteries: present and future journal, January 2017

Superionic glass-ceramic electrolytes for room-temperature rechargeable sodium batteries journal, January 2012

Sulfide Glass-Ceramic Electrolytes for All-Solid-State Lithium and Sodium Batteries journal, July 2014

Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na 3 PSe 4 journal, December 2015

Na 3 PSe 4 : A Novel Chalcogenide Solid Electrolyte with High Ionic Conductivity journal, October 2015

An Air-Stable Na 3 SbS 4 Superionic Conductor Prepared by a Rapid and Economic Synthetic Procedure journal, June 2016

Design and synthesis of the superionic conductor Na10SnP2S12 journal, March 2016

Fast ion motion in glassy and amorphous materials journal, December 1983

Fast ion conducting glasses journal, August 1985

Transport studies on mechanochemically synthesized amorphous AgI–Ag2 O–CrO3 superionic system journal, April 2003

Phase transition and the Ag + -ion diffusion in AgI: Effect of homovalent Br − -ion substitution journal, June 1981

Ionic conductivity of glasses in the MI+M2S+(0.1Ga2S3+0.9GeS2) system (M=Li, Na, K and Cs) journal, January 2008

Development of Sulfide Solid Electrolytes and Interface Formation Processes for Bulk-Type All-Solid-State Li and Na Batteries journal, July 2016

Recent progress of glass and glass-ceramics as solid electrolytes for lithium secondary batteries journal, October 2006

Structural investigations of yNa2S+(1−y)PS5/2 glasses using Raman and infrared spectroscopies journal, December 2012

Preparation and characterization of highly sodium ion conducting Na 3 PS 4 –Na 4 SiS 4 solid electrolytes journal, January 2014

High lithium ion conducting glass-ceramics in the system Li2S–P2S5 journal, October 2006

A sulphide lithium super ion conductor is superior to liquid ion conductors for use in rechargeable batteries journal, January 2014

Calculation of Activation Energy of Ionic Conductivity in Silica Glasses by Classical Methods journal, December 1954

Glasses as solid electrolytes journal, May 1980

Ionic Conductivity of Mixed Glass Former 0.35Na 2 O + 0.65[ x B 2 O 3 + (1 – x )P 2 O 5 ] Glasses journal, December 2013

Activation Enthalpy for Diffusion in Glass journal, October 1986

Lithium and sodium battery cathode materials: computational insights into voltage, diffusion and nanostructural properties journal, January 2014

Sodium Ion Diffusion and Voltage Trends in Phosphates Na 4 M 3 (PO 4 ) 2 P 2 O 7 (M = Fe, Mn, Co, Ni) for Possible High-Rate Cathodes journal, June 2015

Design of Li 1+2x Zn 1−x PS 4 , a new lithium ion conductor journal, January 2016

Structural and Na-ion conduction characteristics of Na 3 PS x Se 4−x journal, January 2016

Interface Stability in Solid-State Batteries journal, December 2015

State of the Art and Future Research Needs for Multiscale Analysis of Li-Ion Cells journal, May 2017

Molecular Dynamics Simulation of the Effect of Crystal Orientation on Lithium‐Ion Diffusion at the V 2 O 5 / Li2SiO3 Interface journal, March 1999

Lithium Ion Diffusion Mechanism in Lithium Lanthanum Titanate Solid-State Electrolytes from Atomistic Simulations journal, November 2014

High power lithium ion battery materials by computational design journal, July 2011

A combined molecular dynamics simulation, experimental and coupling model study of the ion dynamics in glassy ionic conductors journal, April 2003

Molecular dynamics simulations of structural changes in mixed alkali (Li–K) silicate glasses journal, September 1999

A new interpretation of the dynamic structure model of ion transport in molten and solid glasses journal, January 2004

Complete Identification of Alkali Sites in Ion Conducting Lithium Silicate Glasses: A Computer Study of Ion Dynamics journal, May 2003

Quickstep: Fast and accurate density functional calculations using a mixed Gaussian and plane waves approach journal, April 2005

cp2k: atomistic simulations of condensed matter systems journal, June 2013

Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases journal, September 2007

Molecular dynamics studies of the vitreous state: Simple ionic systems and silica journal, August 1976

A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal, December 2000

Nudged-elastic band method with two climbing images: Finding transition states in complex energy landscapes journal, January 2015

Optimization methods for finding minimum energy paths journal, April 2008

The classical equation of state of gaseous helium, neon and argon journal, October 1938

New interatomic potential parameters for molecular dynamics simulations of rare-earth (RE = La, Y, Lu, Sc) aluminosilicate glass structures: exploration of RE3+ field-strength effects journal, January 2013

A New Self-Consistent Empirical Interatomic Potential Model for Oxides, Silicates, and Silica-Based Glasses journal, June 2006

Shell-model molecular dynamics calculations of modified silicate glasses journal, March 2006

Molecular dynamics study of Li2SiS3 glass journal, October 1996

Fast Parallel Algorithms for Short-Range Molecular Dynamics journal, March 1995

Li + Cation Environment, Transport, and Mechanical Properties of the LiTFSI Doped N -Methyl- N -alkylpyrrolidinium + TFSI - Ionic Liquids journal, August 2006

Area detector corrections for high quality synchrotron X-ray structure factor measurements journal, January 2012

Two-dimensional detector software: From real detector to idealised image or two-theta scan journal, January 1996

PDFgetX2: a GUI-driven program to obtain the pair distribution function from X-ray powder diffraction data journal, July 2004

Short range order characterization of the Na2S + SiS2 glass system using Raman, infrared and 29Si magic angle spinning nuclear magnetic resonance spectroscopies journal, September 2017

Lattice dynamics of Na 2 S journal, October 1980

Recent Research on Strategies to Improve Ion Conduction in Alkali Metal‐Ion Batteries journal, April 2019

Title: Molecular Dynamics Modeling of the Structure and Na⁺-Ion Transport in Na₂S + SiS₂ Glassy Electrolytes

Electrical Energy Storage for the Grid: A Battery of Choices
journal, November 2011

Basic Research Needs for Electrical Energy Storage. Report of the Basic Energy Sciences Workshop on Electrical Energy Storage, April 2-4, 2007
report, April 2007

Advances and challenges of sodium ion batteries as post lithium ion batteries
journal, January 2015

Current trends and future challenges of electrolytes for sodium-ion batteries
journal, January 2016

Main Challenges for High Performance NAS Battery: Materials and Interfaces
journal, May 2012

Research Development on Sodium-Ion Batteries
journal, October 2014

Sodium and sodium-ion energy storage batteries
journal, August 2012

Parametric study of dry coating process of electrode particle with model material of sulfide solid electrolytes for all-solid-state battery
journal, January 2017

Room-temperature stationary sodium-ion batteries for large-scale electric energy storage
journal, January 2013

Sodium-ion batteries: present and future
journal, January 2017

Superionic glass-ceramic electrolytes for room-temperature rechargeable sodium batteries
journal, January 2012

Sulfide Glass-Ceramic Electrolytes for All-Solid-State Lithium and Sodium Batteries
journal, July 2014

Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na ₃ PSe ₄
journal, December 2015

Na ₃ PSe ₄ : A Novel Chalcogenide Solid Electrolyte with High Ionic Conductivity
journal, October 2015

An Air-Stable Na ₃ SbS ₄ Superionic Conductor Prepared by a Rapid and Economic Synthetic Procedure
journal, June 2016

Design and synthesis of the superionic conductor Na10SnP2S12
journal, March 2016

Fast ion motion in glassy and amorphous materials
journal, December 1983

Fast ion conducting glasses
journal, August 1985

Transport studies on mechanochemically synthesized amorphous AgI–Ag2 O–CrO3 superionic system
journal, April 2003

Phase transition and the ${Ag}^{+}$ -ion diffusion in AgI: Effect of homovalent ${Br}^{-}$ -ion substitution
journal, June 1981

Ionic conductivity of glasses in the MI+M2S+(0.1Ga2S3+0.9GeS2) system (M=Li, Na, K and Cs)
journal, January 2008

Development of Sulfide Solid Electrolytes and Interface Formation Processes for Bulk-Type All-Solid-State Li and Na Batteries
journal, July 2016

Recent progress of glass and glass-ceramics as solid electrolytes for lithium secondary batteries
journal, October 2006

Structural investigations of yNa2S+(1−y)PS5/2 glasses using Raman and infrared spectroscopies
journal, December 2012

Preparation and characterization of highly sodium ion conducting Na ₃ PS ₄ –Na ₄ SiS ₄ solid electrolytes
journal, January 2014

High lithium ion conducting glass-ceramics in the system Li2S–P2S5
journal, October 2006

A sulphide lithium super ion conductor is superior to liquid ion conductors for use in rechargeable batteries
journal, January 2014

Calculation of Activation Energy of Ionic Conductivity in Silica Glasses by Classical Methods
journal, December 1954

Glasses as solid electrolytes
journal, May 1980

Ionic Conductivity of Mixed Glass Former 0.35Na ₂ O + 0.65[ x B ₂ O ₃ + (1 – x )P ₂ O ₅ ] Glasses
journal, December 2013

Activation Enthalpy for Diffusion in Glass
journal, October 1986

Lithium and sodium battery cathode materials: computational insights into voltage, diffusion and nanostructural properties
journal, January 2014

Sodium Ion Diffusion and Voltage Trends in Phosphates Na ₄ M ₃ (PO ₄ ) ₂ P ₂ O ₇ (M = Fe, Mn, Co, Ni) for Possible High-Rate Cathodes
journal, June 2015

Design of Li _1+2x Zn _1−x PS ₄ , a new lithium ion conductor
journal, January 2016

Structural and Na-ion conduction characteristics of Na ₃ PS _x Se _4−x
journal, January 2016

Interface Stability in Solid-State Batteries
journal, December 2015

State of the Art and Future Research Needs for Multiscale Analysis of Li-Ion Cells
journal, May 2017

Molecular Dynamics Simulation of the Effect of Crystal Orientation on Lithium‐Ion Diffusion at the V 2 O 5 / Li2SiO3 Interface
journal, March 1999

Lithium Ion Diffusion Mechanism in Lithium Lanthanum Titanate Solid-State Electrolytes from Atomistic Simulations
journal, November 2014

High power lithium ion battery materials by computational design
journal, July 2011

A combined molecular dynamics simulation, experimental and coupling model study of the ion dynamics in glassy ionic conductors
journal, April 2003

Molecular dynamics simulations of structural changes in mixed alkali (Li–K) silicate glasses
journal, September 1999

A new interpretation of the dynamic structure model of ion transport in molten and solid glasses
journal, January 2004

Complete Identification of Alkali Sites in Ion Conducting Lithium Silicate Glasses: A Computer Study of Ion Dynamics
journal, May 2003

Quickstep: Fast and accurate density functional calculations using a mixed Gaussian and plane waves approach
journal, April 2005

cp2k: atomistic simulations of condensed matter systems
journal, June 2013

Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases
journal, September 2007

Molecular dynamics studies of the vitreous state: Simple ionic systems and silica
journal, August 1976

A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

Nudged-elastic band method with two climbing images: Finding transition states in complex energy landscapes
journal, January 2015

Optimization methods for finding minimum energy paths
journal, April 2008

The classical equation of state of gaseous helium, neon and argon
journal, October 1938

New interatomic potential parameters for molecular dynamics simulations of rare-earth (RE = La, Y, Lu, Sc) aluminosilicate glass structures: exploration of RE3+ field-strength effects
journal, January 2013

A New Self-Consistent Empirical Interatomic Potential Model for Oxides, Silicates, and Silica-Based Glasses
journal, June 2006

Shell-model molecular dynamics calculations of modified silicate glasses
journal, March 2006

Molecular dynamics study of Li2SiS3 glass
journal, October 1996

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

Li ⁺ Cation Environment, Transport, and Mechanical Properties of the LiTFSI Doped N -Methyl- N -alkylpyrrolidinium ⁺ TFSI ^- Ionic Liquids
journal, August 2006

Area detector corrections for high quality synchrotron X-ray structure factor measurements
journal, January 2012

Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996

PDFgetX2: a GUI-driven program to obtain the pair distribution function from X-ray powder diffraction data
journal, July 2004

Short range order characterization of the Na2S + SiS2 glass system using Raman, infrared and 29Si magic angle spinning nuclear magnetic resonance spectroscopies
journal, September 2017

Lattice dynamics of Na ₂ S
journal, October 1980

Recent Research on Strategies to Improve Ion Conduction in Alkali Metal‐Ion Batteries
journal, April 2019