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Nano Research 2023, 16(6): 8433-8447 https://doi.org/10.1007/s12274-022-5364-5
Research Article | Open Access | Issue | Published: 05 March 2023

Current collectors based on multiwalled carbon-nanotubes and few-layer graphene for enhancing the conversion process in scalable lithium-sulfur battery

Show Author's Information Vittorio Marangon1,2,  Edoardo Barcaro2,  Luca Minnetti1,  Wolfgang Brehm3,  Francesco Bonaccorso1,3,  Vittorio Pellegrini1,3,  Jusef Hassoun1,2,4( )
Graphene Labs, Istituto Italiano di Tecnologia, Genoa 16163, Italy
Department of Chemical, Pharmaceutical and Agricultural Sciences, University of Ferrara, Ferrara 44121, Italy
BeDimensional S.p.A., Genoa 16163, Italy
National Interuniversity Consortium of Materials Science and Technology (INSTM), University of Ferrara Research Unit, Ferrara 44121, Italy
Keywords:
carbon nanotubes, scalability, lithium-sulfur battery, few-layer graphene, current collector, sulfur loading
Topics:
Lithium sulfur batteries
Cite this article:
Marangon V, Barcaro E, Minnetti L, et al. Current collectors based on multiwalled carbon-nanotubes and few-layer graphene for enhancing the conversion process in scalable lithium-sulfur battery. Nano Research, 2023, 16(6): 8433-8447. https://doi.org/10.1007/s12274-022-5364-5
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Abstract Full text Electronic supplementary material About this article

We investigated herein the morphological, structural, and electrochemical features of electrodes using a sulfur (S)-super P carbon (SPC) composite (i.e., S@SPC-73), and including few-layer graphene (FLG), multiwalled carbon nanotubes (MWCNTs), or a mixture of them within the current collector design. Furthermore, we studied the effect of two different electron-conducting agents, that is, SPC and FLG, used in the slurry for the electrode preparation. The supports have high structural crystallinity, while their morphologies are dependent on the type of material used. Cyclic voltammetry (CV) shows a reversible and stable conversion reaction between Li and S with an activation process upon the first cycle leading to the decrease of cell polarization. This activation process is verified by electrochemical impedance spectroscopy (EIS) with a decrease of the resistance after the first CV scan. Furthermore, CV at increasing scan rates indicates a Li+ diffusion coefficient (D) ranging between 10−9 and 10−7 cm2·s−1 in the various states of charge of the cell, and the highest D value for the electrodes using FLG as electron-conducting agent. Galvanostatic tests performed at constant current of C/5 (1 C = 1675 mA·gS−1) show high initial specific capacity values, which decrease during the initial cycles due to a partial loss of the active material, and subsequently increase due to the activation process. All the electrodes show a Coulombic efficiency higher than 97% upon the initial cycles, and a retention strongly dependent on the electrode formulation. Therefore, this study suggests a careful control of the electrode in terms of current collector design and slurry composition to achieve good electrode morphology, mechanical stability, and promising electrochemical performance in practical Li-S cells.


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Electronic supplementary material
About this article

Current collectors based on multiwalled carbon-nanotubes and few-layer graphene for enhancing the conversion process in scalable lithium-sulfur battery

Show Author's information Vittorio Marangon1,2, Edoardo Barcaro2, Luca Minnetti1, Wolfgang Brehm3, Francesco Bonaccorso1,3, Vittorio Pellegrini1,3, Jusef Hassoun1,2,4( )
Graphene Labs, Istituto Italiano di Tecnologia, Genoa 16163, Italy
Department of Chemical, Pharmaceutical and Agricultural Sciences, University of Ferrara, Ferrara 44121, Italy
BeDimensional S.p.A., Genoa 16163, Italy
National Interuniversity Consortium of Materials Science and Technology (INSTM), University of Ferrara Research Unit, Ferrara 44121, Italy

Abstract

We investigated herein the morphological, structural, and electrochemical features of electrodes using a sulfur (S)-super P carbon (SPC) composite (i.e., S@SPC-73), and including few-layer graphene (FLG), multiwalled carbon nanotubes (MWCNTs), or a mixture of them within the current collector design. Furthermore, we studied the effect of two different electron-conducting agents, that is, SPC and FLG, used in the slurry for the electrode preparation. The supports have high structural crystallinity, while their morphologies are dependent on the type of material used. Cyclic voltammetry (CV) shows a reversible and stable conversion reaction between Li and S with an activation process upon the first cycle leading to the decrease of cell polarization. This activation process is verified by electrochemical impedance spectroscopy (EIS) with a decrease of the resistance after the first CV scan. Furthermore, CV at increasing scan rates indicates a Li+ diffusion coefficient (D) ranging between 10−9 and 10−7 cm2·s−1 in the various states of charge of the cell, and the highest D value for the electrodes using FLG as electron-conducting agent. Galvanostatic tests performed at constant current of C/5 (1 C = 1675 mA·gS−1) show high initial specific capacity values, which decrease during the initial cycles due to a partial loss of the active material, and subsequently increase due to the activation process. All the electrodes show a Coulombic efficiency higher than 97% upon the initial cycles, and a retention strongly dependent on the electrode formulation. Therefore, this study suggests a careful control of the electrode in terms of current collector design and slurry composition to achieve good electrode morphology, mechanical stability, and promising electrochemical performance in practical Li-S cells.

Keywords: carbon nanotubes, scalability, lithium-sulfur battery, few-layer graphene, current collector, sulfur loading

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Received: 30 August 2022
Revised: 04 November 2022
Accepted: 27 November 2022
Published: 05 March 2023
Issue date: June 2023

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This project/work has received funding from the European Union’s Horizon 2020 research and innovation programme Graphene Flagship (No. 881603). The authors also thank grant “Fondo di Ateneo per la Ricerca Locale (FAR) 2021”, University of Ferrara, and the collaboration project “Accordo di Collaborazione Quadro 2015” between University of Ferrara (Department of Chemical and Pharmaceutical Sciences) and Sapienza University of Rome (Department of Chemistry).

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