Electrochemically primed functional redox mediator generator from the decomposition of solid state electrolyte.

Nat Commun

Chemical Sciences and Engineering Division, Argonne National Laboratory, 9700 Cass Avenue, Lemont, IL, 60439, USA.

Published: April 2019

AI Article Synopsis

  • Recent studies in sulfide-type solid electrolytes have highlighted the oxidative decomposition of phosphorus and sulfur as a key challenge for their practical use in batteries.
  • This research shows that lithium thiophosphate can act as a functional redox mediator to activate commercial lithium sulfide, making it possible to use up to 70 wt.% lithium sulfide in electrodes.
  • The findings reveal that this method improves the activation process and performance of lithium sulfide without being limited by low electrolyte content, demonstrating promising results under stringent testing conditions.

Article Abstract

Recent works into sulfide-type solid electrolyte materials have attracted much attention among the battery community. Specifically, the oxidative decomposition of phosphorus and sulfur based solid state electrolyte has been considered one of the main hurdles towards practical application. Here we demonstrate that this phenomenon can be leveraged when lithium thiophosphate is applied as an electrochemically "switched-on" functional redox mediator-generator for the activation of commercial bulk lithium sulfide at up to 70 wt.% lithium sulfide electrode content. X-ray adsorption near-edge spectroscopy coupled with electrochemical impedance spectroscopy and Raman indicate a catalytic effect of generated redox mediators on the first charge of lithium sulfide. In contrast to pre-solvated redox mediator species, this design decouples the lithium sulfide activation process from the constraints of low electrolyte content cell operation stemming from pre-solvated redox mediators. Reasonable performance is demonstrated at strict testing conditions.

Download full-text PDF

Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6478822PMC
http://dx.doi.org/10.1038/s41467-019-09638-4DOI Listing

Publication Analysis

Top Keywords

lithium sulfide
16
functional redox
8
redox mediator
8
solid state
8
state electrolyte
8
redox mediators
8
pre-solvated redox
8
redox
5
lithium
5
electrochemically primed
4

Similar Publications

Roles of the Polymer Backbone for Sulfurized Polyacrylonitrile Cathodes in Rechargeable Lithium Batteries.

J Am Chem Soc

December 2024

School of Materials Science and Engineering, Department of Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China.

Sulfurized polyacrylonitrile (SPAN) has emerged as a highly promising cathode material for next-generation lithium-sulfur (Li-S) batteries primarily due to its non-polysulfide dissolution and excellent cycle stability. Nevertheless, the specific roles and impacts of the pyrolyzed polyacrylonitrile, which constitutes the polymer backbone of SPAN, remain inadequately understood. In this study, comprehensive investigations from multiple aspects, including electrochemistry, spectroscopy, electron microscopy, and theoretical calculations, were conducted on a series of SPAN materials with various sulfur contents.

View Article and Find Full Text PDF

Structure and property exploration of two-dimensional, bulk, and cluster lithium sulfide using the IMODE method.

Phys Chem Chem Phys

December 2024

Zhejiang Provincial Key Laboratory of Carbon Materials, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, China.

Lithium sulfide (LiS) plays an important role in fields such as energy, environment and semiconductors. Exploration of the microstructure of LiS has significant implications for developing new materials and optimizing related material properties. In this work, the inverse design of materials by the multi-objective differential evolution (IMODE) method combined with density functional theory (DFT) calculations was used to predict the two-dimensional (2D), three-dimensional (3D), and cluster structures of LiS.

View Article and Find Full Text PDF

Graphite (Gr) is the predominant anode material for current lithium-ion technologies. The Gr anode could offer a practical pathway for the development of lithium-sulfur (Li-S) batteries due to its superior stability and safety compared to Li-metal. However, Gr anodes are not compatible with the conventional dilute ether-based electrolytes typically used in Li-S systems.

View Article and Find Full Text PDF

NiCo alloy-decorated nitrogen-doped carbon double-shelled hollow polyhedrons with abundant catalytic active sites to accelerate lithium polysulfides conversion.

J Colloid Interface Sci

February 2025

School of Optoelectronic Science and Engineering, University of Electronic Science and Technology of China, 611731 Chengdu, PR China; Sichuan Province Key Laboratory of Display Science and Technology, Jianshe North Road 4, 610054 Chengdu, PR China; Yibin Institute of UESTC, University of Electronic Science and Technology of China, North Changjiang Road 430, 644005 Yibin, PR China; Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313001, PR China; Kash Institute of Electronics and Information Industry, Kash 844000, PR China; Shenzhen Institute for Advanced Study, UESTC, Shenzhen 518000, PR China. Electronic address:

Lithium-sulfur (Li-S) batteries have received significant attention due to their high theoretical energy density. However, the inherent poor conductivity of S and lithium sulfide (LiS), coupled with the detrimental shuttle effect induced by lithium polysulfides (LiPSs), impedes their commercialization. In this study, we develop NiCo alloy-decorated nitrogen-doped carbon double-shelled hollow polyhedrons (NC/NiCo DSHPs) as highly efficient catalysts for Li-S batteries.

View Article and Find Full Text PDF

A multifunctional self-supporting LLTO/C interlayer for high-performance lithium-sulfur batteries.

Dalton Trans

December 2024

Key Laboratory for Photonic and Electronic Bandgap Materials, Ministry of Education, School of Physics and Electronic Engineering, Harbin Normal University, Harbin 150025, PR China.

Lithium-sulfur (Li-S) batteries are recognized as an encouraging alternative for future power storage technologies. However, their practical application is hindered by several significant challenges, including slow redox kinetics, the shuttle effect, and the formation of lithium dendrites. Here a binder-free, self-supporting multifunctional interlayer composed of lithium lanthanum titanate (LLTO) with amorphous carbon nanofiber matrices for Li-S batteries has been constructed.

View Article and Find Full Text PDF

Want AI Summaries of new PubMed Abstracts delivered to your In-box?

Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!