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      Synthesis of three-dimensionally interconnected sulfur-rich polymers for cathode materials of high-rate lithium–sulfur batteries

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          Abstract

          Elemental sulfur is one of the most attractive cathode active materials in lithium batteries because of its high theoretical specific capacity. Despite the positive aspect, lithium–sulfur batteries have suffered from severe capacity fading and limited rate capability. Here we report facile large-scale synthesis of a class of organosulfur compounds that could open a new chapter in designing cathode materials to advance lithium–sulfur battery technologies. Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases. Our lithium–sulfur cells display discharge capacity of 945 mAh g −1 after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles. Particularly, the organized amine groups in the crystals increase Li +-ion transfer rate, affording a rate performance of 1210, mAh g −1 at 0.1 C and 730 mAh g −1 at 5 C.

          Abstract

          There is intensive research underway into the cathode development of lithium–sulphur batteries. Here, the authors present a battery with organosulfur-containing polymers as the cathode active materials which displays promising electrochemical performance.

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          Most cited references18

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          Graphene anchored with co(3)o(4) nanoparticles as anode of lithium ion batteries with enhanced reversible capacity and cyclic performance.

          We report a facile strategy to synthesize the nanocomposite of Co(3)O(4) nanoparticles anchored on conducting graphene as an advanced anode material for high-performance lithium-ion batteries. The Co(3)O(4) nanoparticles obtained are 10-30 nm in size and homogeneously anchor on graphene sheets as spacers to keep the neighboring sheets separated. This Co(3)O(4)/graphene nanocomposite displays superior Li-battery performance with large reversible capacity, excellent cyclic performance, and good rate capability, highlighting the importance of the anchoring of nanoparticles on graphene sheets for maximum utilization of electrochemically active Co(3)O(4) nanoparticles and graphene for energy storage applications in high-performance lithium-ion batteries.
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            High-performance lithium-ion anodes using a hierarchical bottom-up approach.

            Si-based Li-ion battery anodes have recently received great attention, as they offer specific capacity an order of magnitude beyond that of conventional graphite. The applications of this transformative technology require synthesis routes capable of producing safe and easy-to-handle anode particles with low volume changes and stable performance during battery operation. Herein, we report a large-scale hierarchical bottom-up assembly route for the formation of Si on the nanoscale--containing rigid and robust spheres with irregular channels for rapid access of Li ions into the particle bulk. Large Si volume changes on Li insertion and extraction are accommodated by the particle's internal porosity. Reversible capacities over five times higher than that of the state-of-the-art anodes (1,950 mA h g(-1)) and stable performance are attained. The synthesis process is simple, low-cost, safe and broadly applicable, providing new avenues for the rational engineering of electrode materials with enhanced conductivity and power.
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              Electronically conductive phospho-olivines as lithium storage electrodes.

              Lithium transition metal phosphates have become of great interest as storage cathodes for rechargeable lithium batteries because of their high energy density, low raw materials cost, environmental friendliness and safety. Their key limitation has been extremely low electronic conductivity, until now believed to be intrinsic to this family of compounds. Here we show that controlled cation non-stoichiometry combined with solid-solution doping by metals supervalent to Li+ increases the electronic conductivity of LiFePO4 by a factor of approximately 10(8). The resulting materials show near-theoretical energy density at low charge/discharge rates, and retain significant capacity with little polarization at rates as high as 6,000 mA x g(-1). In a conventional cell design, they may allow development of lithium batteries with the highest power density yet.
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                Author and article information

                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Pub. Group
                2041-1723
                12 June 2015
                2015
                : 6
                : 7278
                Affiliations
                [1 ]Department of Chemistry, Pohang University of Science and Technology (POSTECH) , Pohang 790-784, Korea
                [2 ]Division of Advanced Materials Science, Pohang University of Science and Technology (POSTECH) , Pohang 790-784, Korea
                Author notes
                Article
                ncomms8278
                10.1038/ncomms8278
                4490390
                26065407
                2f709cee-1a5b-4de7-8df0-e7c9bdbdf1a9
                Copyright © 2015, Nature Publishing Group, a division of Macmillan Publishers Limited. All Rights Reserved.

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                : 12 January 2015
                : 24 April 2015
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