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

doi:10.1021/acsami.6b04158

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 journal › Review article › peer-review

64 Scopus citations

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 S^2- 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 language	English (US)
Pages (from-to)	4290-4295
Number of pages	6
Journal	ACS Applied Materials and Interfaces
Volume	9
Issue number	5
DOIs	https://doi.org/10.1021/acsami.6b04158
State	Published - Feb 8 2017

All Science Journal Classification (ASJC) codes

Materials Science(all)

Access to Document

10.1021/acsami.6b04158

Cite this

@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",

note = "Funding Information: This work was supported as part of the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. The NMR, SEM Raman analysis and DFT calculation were performed in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the U.S. Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2017",

month = feb,

day = "8",

doi = "10.1021/acsami.6b04158",

language = "English (US)",

volume = "9",

pages = "4290--4295",

journal = "ACS Applied Materials and Interfaces",

issn = "1944-8244",

publisher = "American Chemical Society",

number = "5",

}

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

N1 - Funding Information: This work was supported as part of the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences. The NMR, SEM Raman analysis and DFT calculation were performed in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the U.S. Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). Publisher Copyright: © 2016 American Chemical Society.

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

SN - 1944-8244

VL - 9

SP - 4290

EP - 4295

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

IS - 5

ER -

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

Abstract

All Science Journal Classification (ASJC) codes

Access to Document

Other files and links

Fingerprint

Cite this