Ammonium Additives to Dissolve Lithium Sulfide through Hydrogen Binding for High-Energy Lithium-Sulfur Batteries

Huilin Pan, Kee Sung Han, M. Vijayakumar, Jie Xiao, Ruiguo Cao, Junzheng Chen, Jiguang Zhang, Karl T. Mueller, Yuyan Shao, Jun Liu

Research output: Contribution to journalReview article

13 Citations (Scopus)

Abstract

In rechargeable Li-S batteries, the uncontrollable passivation of electrodes by highly insulating Li2S limits sulfur utilization, increases polarization, and decreases cycling stability. Dissolving Li2S in organic electrolyte is a facile solution to maintain the active reaction interface between electrolyte and sulfur cathode, and thus address the above issues. Herein, ammonium salts are demonstrated as effective additives to promote the dissolution of Li2S to 1.25 M in DMSO solvent at room temperature. NMR measurements show that the strong hydrogen binding effect of N-H groups plays a critical role in dissolving Li2S by forming complex ligands with S2- anions coupled with the solvent's solvating surrounding. Ammonium additives in electrolyte can also significantly improve the oxidation kinetics of Li2S, and therefore enable the direct use of Li2S as cathode material in Li-S battery system in the future. This provides a new approach to manage the solubility of lithium sulfides through cation coordination with sulfide anion.

Original languageEnglish (US)
Pages (from-to)4290-4295
Number of pages6
JournalACS Applied Materials and Interfaces
Volume9
Issue number5
DOIs
StatePublished - Feb 8 2017

Fingerprint

Ammonium Compounds
Electrolytes
Hydrogen
Lithium
Sulfur
Anions
Cathodes
Negative ions
Sulfides
Dimethyl Sulfoxide
Passivation
Cations
Dissolution
Solubility
Salts
Positive ions
Ligands
Nuclear magnetic resonance
Polarization
Oxidation

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

Cite this

Pan, Huilin ; Han, Kee Sung ; Vijayakumar, M. ; Xiao, Jie ; Cao, Ruiguo ; Chen, Junzheng ; Zhang, Jiguang ; Mueller, Karl T. ; Shao, Yuyan ; Liu, Jun. / Ammonium Additives to Dissolve Lithium Sulfide through Hydrogen Binding for High-Energy Lithium-Sulfur Batteries. In: ACS Applied Materials and Interfaces. 2017 ; Vol. 9, No. 5. pp. 4290-4295.
@article{60da902981544adf8570c256572e3c89,
title = "Ammonium Additives to Dissolve Lithium Sulfide through Hydrogen Binding for High-Energy Lithium-Sulfur Batteries",
abstract = "In rechargeable Li-S batteries, the uncontrollable passivation of electrodes by highly insulating Li2S limits sulfur utilization, increases polarization, and decreases cycling stability. Dissolving Li2S in organic electrolyte is a facile solution to maintain the active reaction interface between electrolyte and sulfur cathode, and thus address the above issues. Herein, ammonium salts are demonstrated as effective additives to promote the dissolution of Li2S to 1.25 M in DMSO solvent at room temperature. NMR measurements show that the strong hydrogen binding effect of N-H groups plays a critical role in dissolving Li2S by forming complex ligands with S2- anions coupled with the solvent's solvating surrounding. Ammonium additives in electrolyte can also significantly improve the oxidation kinetics of Li2S, and therefore enable the direct use of Li2S as cathode material in Li-S battery system in the future. This provides a new approach to manage the solubility of lithium sulfides through cation coordination with sulfide anion.",
author = "Huilin Pan and Han, {Kee Sung} and M. Vijayakumar and Jie Xiao and Ruiguo Cao and Junzheng Chen and Jiguang Zhang and Mueller, {Karl T.} and Yuyan Shao and Jun Liu",
year = "2017",
month = "2",
day = "8",
doi = "10.1021/acsami.6b04158",
language = "English (US)",
volume = "9",
pages = "4290--4295",
journal = "ACS applied materials & interfaces",
issn = "1944-8244",
publisher = "American Chemical Society",
number = "5",

}

Pan, H, Han, KS, Vijayakumar, M, Xiao, J, Cao, R, Chen, J, Zhang, J, Mueller, KT, Shao, Y & Liu, J 2017, 'Ammonium Additives to Dissolve Lithium Sulfide through Hydrogen Binding for High-Energy Lithium-Sulfur Batteries', ACS Applied Materials and Interfaces, vol. 9, no. 5, pp. 4290-4295. https://doi.org/10.1021/acsami.6b04158

Ammonium Additives to Dissolve Lithium Sulfide through Hydrogen Binding for High-Energy Lithium-Sulfur Batteries. / Pan, Huilin; Han, Kee Sung; Vijayakumar, M.; Xiao, Jie; Cao, Ruiguo; Chen, Junzheng; Zhang, Jiguang; Mueller, Karl T.; Shao, Yuyan; Liu, Jun.

In: ACS Applied Materials and Interfaces, Vol. 9, No. 5, 08.02.2017, p. 4290-4295.

Research output: Contribution to journalReview article

TY - JOUR

T1 - Ammonium Additives to Dissolve Lithium Sulfide through Hydrogen Binding for High-Energy Lithium-Sulfur Batteries

AU - Pan, Huilin

AU - Han, Kee Sung

AU - Vijayakumar, M.

AU - Xiao, Jie

AU - Cao, Ruiguo

AU - Chen, Junzheng

AU - Zhang, Jiguang

AU - Mueller, Karl T.

AU - Shao, Yuyan

AU - Liu, Jun

PY - 2017/2/8

Y1 - 2017/2/8

N2 - In rechargeable Li-S batteries, the uncontrollable passivation of electrodes by highly insulating Li2S limits sulfur utilization, increases polarization, and decreases cycling stability. Dissolving Li2S in organic electrolyte is a facile solution to maintain the active reaction interface between electrolyte and sulfur cathode, and thus address the above issues. Herein, ammonium salts are demonstrated as effective additives to promote the dissolution of Li2S to 1.25 M in DMSO solvent at room temperature. NMR measurements show that the strong hydrogen binding effect of N-H groups plays a critical role in dissolving Li2S by forming complex ligands with S2- anions coupled with the solvent's solvating surrounding. Ammonium additives in electrolyte can also significantly improve the oxidation kinetics of Li2S, and therefore enable the direct use of Li2S as cathode material in Li-S battery system in the future. This provides a new approach to manage the solubility of lithium sulfides through cation coordination with sulfide anion.

AB - In rechargeable Li-S batteries, the uncontrollable passivation of electrodes by highly insulating Li2S limits sulfur utilization, increases polarization, and decreases cycling stability. Dissolving Li2S in organic electrolyte is a facile solution to maintain the active reaction interface between electrolyte and sulfur cathode, and thus address the above issues. Herein, ammonium salts are demonstrated as effective additives to promote the dissolution of Li2S to 1.25 M in DMSO solvent at room temperature. NMR measurements show that the strong hydrogen binding effect of N-H groups plays a critical role in dissolving Li2S by forming complex ligands with S2- anions coupled with the solvent's solvating surrounding. Ammonium additives in electrolyte can also significantly improve the oxidation kinetics of Li2S, and therefore enable the direct use of Li2S as cathode material in Li-S battery system in the future. This provides a new approach to manage the solubility of lithium sulfides through cation coordination with sulfide anion.

UR - http://www.scopus.com/inward/record.url?scp=85011954452&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85011954452&partnerID=8YFLogxK

U2 - 10.1021/acsami.6b04158

DO - 10.1021/acsami.6b04158

M3 - Review article

C2 - 27367455

AN - SCOPUS:85011954452

VL - 9

SP - 4290

EP - 4295

JO - ACS applied materials & interfaces

JF - ACS applied materials & interfaces

SN - 1944-8244

IS - 5

ER -