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Structural origins of enhanced capacity retention in novel copolymerized sulfur-based composite cathodes for high-energy density Li-S batteries

  • Polymers/Soft Matter Prospective Article
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Abstract

Poly[sulfur-random-1,3-diisopropenylbenzene (DIB)] copolymers synthesized via inverse vulcanization form electrochemically active polymers used as cathodes for high-energy density Li-S batteries, capable of enhanced capacity retention (1005 mAh/g at 100 cycles) and lifetimes of over 500 cycles. In this prospective, we demonstrate how analytical electron microscopy can be employed as a powerful tool to explore the origins of the enhanced capacity retention. We analyze morphological and compositional features when the copolymers, with DIB contents up to 50% by mass, are blended with carbon nanoparticles. Replacing the elemental sulfur with the copolymers improves the compatibility and interfacial contact between active sulfur compounds and conductive carbons. There also appears to be improvements of the cathode mechanical stability that leads to less cracking but preserving porosity. This compatibilization scheme through stabilized organosulfur copolymers represents an alternative strategy to the nanoscale encapsulation schemes which are often used to improve the cycle life in high-energy density Li-S batteries.

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Acknowledgments

The authors acknowledge the ACS-PRF (51026-ND10), the NSF (CHE-1305773), the WCU Program through the NRF of Korea funded by the Ministry of Education, Science and Technology (R31-10013) for support of this work. V.P.O. acknowledges the support by National Institute of Standards and Technology (Award No 70NANB12H164). K.C. acknowledges the support from NRF for the National Creative Research Initiative Center for Intelligent Hybrids (2010-0018290).

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Authors and Affiliations

  1. Materials Science and Engineering Division, Materials Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, Maryland, 20899, USA

    Vladimir P. Oleshko, Jenny Kim, Jennifer L. Schaefer, Steven D. Hudson & Christopher L. Soles

  2. Department of Chemistry and Biochemistry, University of Arizona, Tucson, Arizona, 8721, USA

    Adam G. Simmonds, Jared J. Griebel, Richard S. Glass & Jeffrey Pyun

  3. Department of Chemical and Biological Engineering, The World Class University Program of Chemical Convergence for Energy and Environment, The National Creative Research Initiative Centerfor Intelligent Hybrids, and Centerfor Nanoparticle Research, Institute for Basic Research, Seoul National University, Seoul, 151-744, Korea

    Jared J. Griebel, Kookheon Char & Jeffrey Pyun

  4. University of Maryland, College Park, Maryland, 20742, USA

    Vladimir P. Oleshko

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  1. Vladimir P. Oleshko
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Correspondence to Vladimir P. Oleshko.

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Oleshko, V.P., Kim, J., Schaefer, J.L. et al. Structural origins of enhanced capacity retention in novel copolymerized sulfur-based composite cathodes for high-energy density Li-S batteries. MRS Communications 5, 353–364 (2015). https://doi.org/10.1557/mrc.2015.41

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