The Importance of Confined Sulfur Nanodomains and Adjoining Electron Conductive Pathways in Subreaction Regimes of Li‐S Batteries |
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Authors: | Jungjin Park Eui Tae Kim Chunjoong Kim Jeffrey Pyun Hyung‐Seok Jang Jaeho Shin Jang Wook Choi Kookheon Char Yung‐Eun Sung |
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Institution: | 1. Graduate School of EEWS (Energy, Environment, Water, Sustainability), Korea Advanced Institute of Science and Technology (KAIST), Daejeon, Republic of Korea;2. School of Chemical and Biological Engineering, Seoul National University, Seoul, Republic of Korea;3. Center for Nanoparticle Research, Institute for Basic Science, Seoul, Republic of Korea;4. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, USA;5. The National Creative Research Initiative Center for Intelligent Hybrids, Gwanak‐gu, Seoul, Republic of Korea;6. Department of Material Science and Engineering, Chungnam National University, Daejeon, Republic of Korea;7. Department of Chemistry and Biochemistry, University of Arizona, Tucson, AZ, USA |
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Abstract: | Polysulfide dissolution into the electrolyte and poor electric conductivity of elemental sulfur are well‐known origins for capacity fading in lithium–sulfur batteries. Various smart electrode designs have lately been introduced to avoid these fading mechanisms, most of which demonstrate significantly improved cycle life. Nevertheless, an in‐depth understanding on the effect of sulfur microstructure and nanoscale electron transport near sulfur is currently lacking. In this study, the authors report an organized nanocomposite comprising linear sulfur chains and oleylamine‐functionalized reduced graphene oxide (O‐rGO) to achieve robust cycling performance (81.7% retention after 500 cycles) as well as to investigate the reaction mechanism in different regimes, i.e., S8 dissolution, polysulfide conversion, and Li2S formation. In the nanocomposite, linear sulfur chains terminate with 1,3‐diisopropylbenzene are covalently linked to O‐rGO. The comparison with control samples that do not contain either the capping of sulfur chains or O‐rGO reveals the synergistic interplay between both treatments, simultaneously unveiling the distinct roles of confined sulfur nanodomains and their adjoining electron pathways in different reaction regimes. |
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Keywords: | capping agents electrochemical analyses lithium‐sulfur batteries polysulfide kinetics sulfur‐carbon copolymers |
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