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Title: Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries

; ; ;  [1]
  1. (Waterloo)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
OSTI Identifier:
Resource Type:
Journal Article
Resource Relation:
Journal Name: Nat. Commun.; Journal Volume: 5; Journal Issue: 08, 2014
Country of Publication:
United States

Citation Formats

Pang, Quan, Kundu, Dipan, Cuisinier, Marine, and Nazar, L.F.. Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries. United States: N. p., 2014. Web. doi:10.1038/ncomms5759.
Pang, Quan, Kundu, Dipan, Cuisinier, Marine, & Nazar, L.F.. Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries. United States. doi:10.1038/ncomms5759.
Pang, Quan, Kundu, Dipan, Cuisinier, Marine, and Nazar, L.F.. Tue . "Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries". United States. doi:10.1038/ncomms5759.
title = {Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries},
author = {Pang, Quan and Kundu, Dipan and Cuisinier, Marine and Nazar, L.F.},
abstractNote = {},
doi = {10.1038/ncomms5759},
journal = {Nat. Commun.},
number = 08, 2014,
volume = 5,
place = {United States},
year = {Tue Aug 26 00:00:00 EDT 2014},
month = {Tue Aug 26 00:00:00 EDT 2014}
  • Lithium-sulphur batteries have high theoretical energy density and potentially low cost, but significant challenges such as severe capacity degradation prevent its widespread adoption. Here we report a new design of lithium-sulphur battery using electrically connected graphite and lithium metal as a hybrid anode to control undesirable surface reactions on lithium. Lithiated graphite placed in front of the lithium metal functions as an artificial, self-regulated solid electrolyte interface layer to actively control the electrochemical reactions and minimize the deleterious side reactions, leading to significant performance improvements. Lithium-sulphur cells incorporating this hybrid anodes deliver capacities of >800 mAhg(-1) for 400 cycles atmore » a high rate of 1,737mAg(-1), with only 11% capacity fade and a Coulombic efficiency >99%. This simple hybrid concept may also provide scientific strategies for protecting metal anodes in other energy-storage devices.« less
  • Lithium sulfur (Li-S) redox flow battery (RFB) is a promising candidate for high energy large-scale energy storage application due to good solubility of long-chain polysulfide species and low cost of sulfur. In this report, recent progress and new concepts for Li-S redox flow batteries are discussed with an emphasis on the fundamental understanding and control of lithium polysulfide chemistry to enable the development of liquid phase Li-S redox flow prototype cells. These differ significantly from conventional static Li-S batteries targeting for vehicle electrification. A high solubility of the different lithium polysulfides generated at different depths of discharge and states ofmore » charge is required for a flow battery in order to take full advantage of the multiple electron transitions between elemental sulfur and Li2S. A new DMSO-based electrolyte is proposed for Li-S redox flow batteries, which not only enables the high solubility of lithium polysulfide species, especially for the short-chain species, but also results in excellent cycling with a high Coulombic efficiency. The challenges and opportunities for the Li-S redox flow concept have also been discussed in depth.« less
  • Lithium electrodes in a few selected polar aprotic electrolyte systems were investigated using electrochemical techniques in conjunction with surface - sensitive Fourier transform infrared spectroscopy and scanning electron microscopy. The solvents used were {gamma} butyrolactone (BL), propylene carbonate (PC), and tetrahydrofuran (THF), and the salts included LiClO{sub 4} and LiAsF{sub 6}. Cycling efficiency of lithium electrodes was correlated to their surface chemistry and morphology in the various solvent systems. The effects of both water and oxygen contamination were rigorously studied. It was found that the presence of oxygen in solutions considerably increased the cycling efficiency of the lithium electrode. Thismore » effect correlates well with the influence of the presence of oxygen on the surface morphology of lithium electrodes in solutions. The presence of water increases cycling efficiency of Li electrodes in PC, and decreases cycling efficiency of Li electrodes in ethers. These results are discussed in light of the surface chemistry of lithium in the various solvent systems.« less
  • Water is generally considered to be deteriorating to the performance of aprotic Li-air batteries, while it is challenged by the disparate effects observed recently. This has provoked a range of discussion on the role of water and its impact on the battery operation. In this work, a distinct battery chemistry that prevails in water-contaminated aprotic Li-O 2 batteries was discovered. Both lithium ions and protons were found to be involved in the oxygen reduction (ORR) and evolution reactions (OER), and LiOOH and LiOH were identified as predominant materials in the discharge product. As a new lithium compound, the crystallographic andmore » spectroscopic characteristics of LiOOH∙H 2O were scrutinized both experimentally and theoretically. The structure of LiOOH∙H 2O was found to be closely related to that of LiOH∙H 2O implying a fast conversion kinetics between the two phases. Intriguingly, LiOOH∙H 2O exhibits superior dynamic property towards the reaction with I 3 -, which renders considerably lower overpotential during the charging process. We anticipate that the new battery chemistry unveiled in this mechanistic study would provide important insights to the understanding of nominally aprotic Li-O 2 batteries and help to tackle the critical issues confronted.« less