Adsorption Mechanisms of Lithium Polysulfides on Graphene-Based Interlayers in Lithium Sulfur Batteries

Chi You Liu, Elise Y. Li

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

One of the most critical problems in lithium-sulfur (Li-S) batteries is the shuttle effect. The transfer of soluble lithium polysulfides (LiPSs) from the sulfur cathode to the lithium anode leads to a degradation in Li-S battery capacity and life cycles. Recent studies reveal that the carbon-based interlayer materials introduced between the cathode and anode can effectively improve the shuttle effect problem and increase the battery life cycles. In this work, different types of the N-doped, S-doped, and N,S-codoped graphene surfaces are investigated by theoretical calculations. We find that a strong interaction may exist between some of the heteroatom-doped graphene surfaces and lithium ions, and that the adsorption of LiPSs may proceed via one of the three mechanisms, the dissociative, the destructive, and the intact adsorptions. Detailed structural and electronic analyses indicate that the Li-trapped N,S-codoped graphene interlayers (NSG1 and NSG2) could efficiently reduce the shuttle effect through the intact adsorption mechanism. Our results provide a plausible explanation for the observed better performance of the N,S-codoped graphene interlayers in Li-S batteries.

Original languageEnglish
Pages (from-to)455-463
Number of pages9
JournalACS Applied Energy Materials
Volume1
Issue number2
DOIs
Publication statusPublished - 2018 Feb 26

Fingerprint

Polysulfides
Graphite
Lithium
Graphene
Adsorption
Life cycle
Anodes
Cathodes
Sulfur
Carbon
Ions
Degradation
Lithium sulfur batteries
polysulfide

Keywords

  • DFT calculation
  • Li-S battery
  • VASP
  • heteroatom-doped graphene
  • lithium polysulfides
  • shuttle effect

ASJC Scopus subject areas

  • Energy Engineering and Power Technology
  • Chemical Engineering (miscellaneous)
  • Electrochemistry
  • Materials Chemistry
  • Electrical and Electronic Engineering

Cite this

Adsorption Mechanisms of Lithium Polysulfides on Graphene-Based Interlayers in Lithium Sulfur Batteries. / Liu, Chi You; Li, Elise Y.

In: ACS Applied Energy Materials, Vol. 1, No. 2, 26.02.2018, p. 455-463.

Research output: Contribution to journalArticle

@article{ff7258a5a09148dd907bc5803b7b7c7f,
title = "Adsorption Mechanisms of Lithium Polysulfides on Graphene-Based Interlayers in Lithium Sulfur Batteries",
abstract = "One of the most critical problems in lithium-sulfur (Li-S) batteries is the shuttle effect. The transfer of soluble lithium polysulfides (LiPSs) from the sulfur cathode to the lithium anode leads to a degradation in Li-S battery capacity and life cycles. Recent studies reveal that the carbon-based interlayer materials introduced between the cathode and anode can effectively improve the shuttle effect problem and increase the battery life cycles. In this work, different types of the N-doped, S-doped, and N,S-codoped graphene surfaces are investigated by theoretical calculations. We find that a strong interaction may exist between some of the heteroatom-doped graphene surfaces and lithium ions, and that the adsorption of LiPSs may proceed via one of the three mechanisms, the dissociative, the destructive, and the intact adsorptions. Detailed structural and electronic analyses indicate that the Li-trapped N,S-codoped graphene interlayers (NSG1 and NSG2) could efficiently reduce the shuttle effect through the intact adsorption mechanism. Our results provide a plausible explanation for the observed better performance of the N,S-codoped graphene interlayers in Li-S batteries.",
keywords = "DFT calculation, Li-S battery, VASP, heteroatom-doped graphene, lithium polysulfides, shuttle effect",
author = "Liu, {Chi You} and Li, {Elise Y.}",
year = "2018",
month = "2",
day = "26",
doi = "10.1021/acsaem.7b00096",
language = "English",
volume = "1",
pages = "455--463",
journal = "ACS Applied Energy Materials",
issn = "2574-0962",
publisher = "American Chemical Society",
number = "2",

}

TY - JOUR

T1 - Adsorption Mechanisms of Lithium Polysulfides on Graphene-Based Interlayers in Lithium Sulfur Batteries

AU - Liu, Chi You

AU - Li, Elise Y.

PY - 2018/2/26

Y1 - 2018/2/26

N2 - One of the most critical problems in lithium-sulfur (Li-S) batteries is the shuttle effect. The transfer of soluble lithium polysulfides (LiPSs) from the sulfur cathode to the lithium anode leads to a degradation in Li-S battery capacity and life cycles. Recent studies reveal that the carbon-based interlayer materials introduced between the cathode and anode can effectively improve the shuttle effect problem and increase the battery life cycles. In this work, different types of the N-doped, S-doped, and N,S-codoped graphene surfaces are investigated by theoretical calculations. We find that a strong interaction may exist between some of the heteroatom-doped graphene surfaces and lithium ions, and that the adsorption of LiPSs may proceed via one of the three mechanisms, the dissociative, the destructive, and the intact adsorptions. Detailed structural and electronic analyses indicate that the Li-trapped N,S-codoped graphene interlayers (NSG1 and NSG2) could efficiently reduce the shuttle effect through the intact adsorption mechanism. Our results provide a plausible explanation for the observed better performance of the N,S-codoped graphene interlayers in Li-S batteries.

AB - One of the most critical problems in lithium-sulfur (Li-S) batteries is the shuttle effect. The transfer of soluble lithium polysulfides (LiPSs) from the sulfur cathode to the lithium anode leads to a degradation in Li-S battery capacity and life cycles. Recent studies reveal that the carbon-based interlayer materials introduced between the cathode and anode can effectively improve the shuttle effect problem and increase the battery life cycles. In this work, different types of the N-doped, S-doped, and N,S-codoped graphene surfaces are investigated by theoretical calculations. We find that a strong interaction may exist between some of the heteroatom-doped graphene surfaces and lithium ions, and that the adsorption of LiPSs may proceed via one of the three mechanisms, the dissociative, the destructive, and the intact adsorptions. Detailed structural and electronic analyses indicate that the Li-trapped N,S-codoped graphene interlayers (NSG1 and NSG2) could efficiently reduce the shuttle effect through the intact adsorption mechanism. Our results provide a plausible explanation for the observed better performance of the N,S-codoped graphene interlayers in Li-S batteries.

KW - DFT calculation

KW - Li-S battery

KW - VASP

KW - heteroatom-doped graphene

KW - lithium polysulfides

KW - shuttle effect

UR - http://www.scopus.com/inward/record.url?scp=85059687796&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85059687796&partnerID=8YFLogxK

U2 - 10.1021/acsaem.7b00096

DO - 10.1021/acsaem.7b00096

M3 - Article

AN - SCOPUS:85059687796

VL - 1

SP - 455

EP - 463

JO - ACS Applied Energy Materials

JF - ACS Applied Energy Materials

SN - 2574-0962

IS - 2

ER -