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Title: Interaction of FeS 2 and Sulfur in Li-S Battery System

Journal Article · · Journal of the Electrochemical Society
 [1];  [2];  [2];  [1];  [1];  [1];  [2];  [2];  [3];  [1]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Stony Brook Univ., NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)

Many transition metal sulfides are electronically conductive, electrochemically active and reversible in reactions with lithium. However, the application of transition metal sulfides as sulfur cathode additives in lithium-sulfur (Li-S) batteries has not been fully explored. In this study, Pyrite (FeS2) is studied as a capacity contributing conductive additive in sulfur cathode for Li-S batteries. Electrochemically discharging the S-FeS2 composite electrodes to 1.0 V activates the FeS2 component, contributing to the improved Li-S cell discharge energy density. However, direct activation of the FeS2 component in a fresh S-FeS2 cell results in a significant shuttling effect in the subsequent charging process, preventing further cell cycling. The slight FeS2 solubility in electrolyte and its activation alone in S-FeS2 cells are not the root causes of the severe shuttling effect. The observed severe shuttling effect is strongly correlated to the 1st charging of the activated S-FeS2 electrode that promotes iron dissolution in electrolyte and the deposition of electronically conductive FeS on the anode SEI. Pre-cycling of the S-FeS2 cell prior to the FeS2 activation or the use of LiNO3 electrolyte additive help to prevent the severe shuttling effect and allow the cell to cycle between 2.6 V to 1.0 V with an extra capacity contribution from the FeS2 components. However, a more effective method of anode pre-passivation is still needed to fully protect the lithium surface from FeS deposition and allow the S-FeS2 electrode to maintain high energy density over extended cycles. A mechanism explaining the observed phenomena based on the experimental data is proposed and discussed

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012704
OSTI ID:
1389218
Report Number(s):
BNL--114124-2017-JA
Journal Information:
Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 1 Vol. 164; ISSN 0013-4651
Publisher:
The Electrochemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (14)

Operando Multi-modal Synchrotron Investigation for Structural and Chemical Evolution of Cupric Sulfide (CuS) Additive in Li-S battery journal October 2017
Heterogeneous/Homogeneous Mediators for High-Energy-Density Lithium-Sulfur Batteries: Progress and Prospects journal June 2018
In Situ Formation of Copper-Based Hosts Embedded within 3D N-Doped Hierarchically Porous Carbon Networks for Ultralong Cycle Lithium-Sulfur Batteries journal August 2018
Enhanced Sulfur Transformation by Multifunctional FeS 2 /FeS/S Composites for High‐Volumetric Capacity Cathodes in Lithium–Sulfur Batteries journal February 2019
Boosting High‐Rate Li–S Batteries by an MOF‐Derived Catalytic Electrode with a Layer‐by‐Layer Structure journal June 2019
Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries journal June 2018
High Capacity All-Solid-State Lithium Batteries Enabled by Pyrite-Sulfur Composites journal July 2018
Defect Control in the Synthesis of 2 D MoS 2 Nanosheets: Polysulfide Trapping in Composite Sulfur Cathodes for Li–S Batteries journal March 2020
Nanocrystalline Pyrite for Photovoltaic Applications journal June 2018
Mechanochemically synthesized pyrite and its electrochemical behavior as cathode for lithium batteries journal May 2019
Operando Multi-modal Synchrotron Investigation for Structural and Chemical Evolution of Cupric Sulfide (CuS) Additive in Li-S battery journal October 2017
Rational design of polar/nonpolar mediators toward efficient sulfur fixation and enhanced conductivity journal January 2020
Ni 3 S 2 anchored to N/S co-doped reduced graphene oxide with highly pleated structure as a sulfur host for lithium–sulfur batteries journal January 2020
Improvement of Li-Sulfur Cell Cycling Performance by Use of Fe 1-x S@NC as a Functional Additive for Chemical Confinement of Lithium Polysulfides journal December 2018

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