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Carbon 122 (2017) 106e113 Contents lists available at ScienceDirect Carbon journal homepage: www.elsevier.com/locate/carbon Graphene-supported highly crosslinked organosulfur nanoparticles as cathode materials for high-rate, long-life lithium-sulfur battery Shuaibo Zeng a, Ligui Li a, b, *, Lihong Xie a, Dengke Zhao a, Ni Zhou a, Nan Wang a, Shaowei Chen a, c, ** a Guangzhou Key Laboratory for Surface Chemistry of Energy Materials, New Energy Research Institute, College of Environment and Energy, South China University of Technology, Guangzhou Higher Education Mega Center, Guangzhou 510006, China b Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, College of Environment and Energy, South China University of Technology, Guangzhou 510006, China c Department of Chemistry and Biochemistry, University of California, 1156 High Street, Santa Cruz, CA 95064, USA articleinfo Article history: Received 31 March 2017 Received in revised form 4 June 2017 Accepted 14 June 2017 Available online 18 June 2017 Keywords: Lithium-sulfur battery Rate performance Cycling stability Sulfur copolymer 1. Introduction Lithium-sulfur (Li-S) batteries are regarded as one of the most promising candidates for next-generation rechargeable batteries due to various unique advantages: (a) the energy density of Li-S batteries (2567 Wh Kg1) is about five times higher than that of conventional Li-ion batteries due to the high specific capacity of sulfur (1672 mAh g1), such that Li-S batteries can meet the ever- increasing power demands in portable electronics and electric ve- hicles [1e3]; (b) sulfur is among the most earth-abundant elements * Corresponding author. Guangzhou Key Laboratory for Surface Chemistry of Energy Materials, New Energy Research Institute, College of Environment and En- ergy, South China University of Technology, Guangzhou Higher Education Mega Center, Guangzhou 510006, China. ** Corresponding author. Department of Chemistry and Biochemistry, University of California, 1156 High Street, Santa Cruz, CA 95064, USA. E-mail addresses: esguili@scut.edu.cn (L. Li), shaowei@ucsc.edu (S. Chen). http://dx.doi.org/10.1016/j.carbon.2017.06.036 0008-6223/© 2017 Elsevier Ltd. All rights reserved. abstract Lithium-sulfur batteries represent one of the next-generation Li-ion batteries; yet rapid performance degradation is a major challenge. Herein, a highly crosslinked copolymer is synthesized through ther- mally activated polymerization of sulfur and trithiocyanuric acid onto the surface of reduced graphene oxide nanosheets. Of the thus-synthesized composites, the sample with a high sulfur content of 81.79 wt.% shows a remarkable rate performance of 1341 mAh g1 at 0.1 C and 861 mAh g1 at 1 C with an almost 100% coulombic efficiency. The composite electrode also effectively impedes the dissolution of polysulfides and their shuttle diffusion because of the abundant and robust chemical bonding between sulfur and trithiocyanuric acid and spatial confinement of polysulfides by the reduced graphene oxide sheets, which leads to 81.72% retention of the initial capacity even after 500 deep charge-discharge cycles at 1 C, corresponding to a decay rate of only 0.0404% per cycle. This performance is markedly better than those of comparative materials prepared in a similar fashion but at either higher or lower S loading, and among the highest in sulfur copolymer cathodes to date. The results provide an effective paradigm in the preparation and engineering of polymer cathode materials for high-performance lithium-sulfur batteries. © 2017 Elsevier Ltd. All rights reserved. and may sustain massive commercialization of Li-S batteries [4,5]; and (c) Li-S batteries are easy to fabricate, cost-effective and envi- ronmentally friendly [6e8]. However, to realize large-scale commercialization of Li-S batteries, several critical issues need to be resolved, such as the low coulombic efficiency and rate capacity resulting from the low electrical conductivity of sulfur and poly- sulfides (~5 1030 S cm1 at 25 C) [9,10], rapid capacity atten- uation caused by mechanical degradation of the cathode due to the large volume expansion (up to 80%) of sulfur lithiation, and the so- called “shuttle” effect of lithium polysulfides (Li2Sn with 4 n 8) due to the dissolution and diffusion of polysulfides in organic electrolytes [11e14]. Moreover, lithium dendrites can be easily formed in the lithium metal anode during charge-discharge pro- cesses, which may short the circuit by penetration into the thin membrane, resulting in a short life-span and serious safety con- cerns [15]. To mitigate these issues, extensive research efforts have been devoted to the design and engineering of novel cathode materialsPDF Image | Graphene-supported highly crosslinked organosulfur nanoparticles as cathode materials
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