Li2S growth on graphene: Impact on the electrochemical performance of Li-S batteries

Longo, Roberto C.; Camacho-Forero, Luis E.; Balbuena, Perla B.

doi:10.1063/1.5135304

Title: Li₂S growth on graphene: Impact on the electrochemical performance of Li-S batteries

Journal Article · 07 January 2020 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5135304 · OSTI ID:1799459

Longo, Roberto C. ^[1];

^[2];

^[2]

Texas A & M Univ., College Station, TX (United States); OSTI
Texas A & M Univ., College Station, TX (United States)

Lithium-sulfur batteries show remarkable potential for energy storage applications due to their high-specific capacity and the low cost of active materials, especially sulfur. However, whereas there is a consensus about the use of lithium metal as the negative electrode, there is not a clear and widely accepted architectural design for the positive electrode of sulfur batteries. The difficulties arise when trying to find a balance between high-surface-area architectures and practical utilization of the sulfur content. Intensive understanding of the interfacial mechanisms becomes then crucial to design optimized carbon-hosted sulfur architectures with enhanced electrochemical performance. In this work, we use density functional theory (DFT)-based first principles calculations to describe and characterize the growing mechanisms of Li₂S active material on graphene, taken as an example of a nonencapsulated carbon host for the positive electrode of Li-S batteries. We first unravel the two growing mechanisms of Li2S supported nanostructures, which explain recent experimental findings on real-time monitoring of interfacial deposition of lithium sulfides during discharge, obtained by means of in situ atomic force microscopy. Then, using a combination of mathematical tools and DFT calculations, we obtain the first cycle voltage plot, explaining the three different regions observed that ultimately lead to the formation of high-order polysulfides upon charge. Finally, we show how the different Li₂S supported nanostructures can be characterized in X-ray photoelectron spectroscopy measurements. Altogether, this work provides useful insights for the rational design of new carbon-hosted sulfur architectures with optimized characteristics for the positive electrode of lithium-sulfur batteries.

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Research Organization:: Texas A & M University, College Station, TX (United States). Texas A & M Engineering Experiment Station

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0008210

OSTI ID:: 1799459

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 1 Vol. 152; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Li2S growth on graphene: Impact on the electrochemical performance of Li-S batteries

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Title: Li₂S growth on graphene: Impact on the electrochemical performance of Li-S batteries