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Freestanding and Sandwich‐Structured Electrode Material with High Areal Mass Loading for Long‐Life Lithium–Sulfur Batteries
Authors:Mingpeng Yu  Junsheng Ma  Ming Xie  Hongquan Song  Fuyang Tian  Shanshan Xu  Yun Zhou  Bei Li  Di Wu  Hong Qiu  Rongming Wang
Affiliation:1. Department of Physics, University of Science and Technology Beijing, Beijing, P. R. China;2. BattFlex Technologies, Inc, Wuhan, P. R. China;3. Institute for Applied Physics, University of Science and Technology Beijing, Beijing, P. R. China;4. College of Chemistry, Chongqing Normal University, Chongqing, P. R. China
Abstract:Freestanding cathode materials with sandwich‐structured characteristic are synthesized for high‐performance lithium–sulfur battery. Sulfur is impregnated in nitrogen‐doped graphene and constructed as primary active material, which is further welded in the carbon nanotube/nanofibrillated cellulose (CNT/NFC) framework. Interconnected CNT/NFC layers on both sides of active layer are uniquely synthesized to entrap polysulfide species and supply efficient electron transport. The 3D composite network creates a hierarchical architecture with outstanding electrical and mechanical properties. Synergistic effects generated from physical and chemical interaction could effectively alleviate the dissolution and shuttling of the polysulfide ions. Theoretical calculations reveal the hydroxyl functionization exhibits a strong chemical binding with the discharge product (i.e., Li2S). Electrochemical measurements suggest that the rationally designed structure endows the electrode with high specific capacity and excellent rate performance. Specifically, the electrode with high areal sulfur loading of 8.1 mg cm?2 exhibits an areal capacity of ≈8 mA h cm?2 and an ultralow capacity fading of 0.067% per cycle over 1000 discharge/charge cycles at C/2 rate, while the average coulombic efficiency is around 97.3%, indicating good electrochemical reversibility. This novel and low‐cost fabrication procedure is readily scalable and provides a promising avenue for potential industrial applications.
Keywords:graphene  hydroxyl functionalization  lithium–  sulfur batteries  sandwich‐structured electrode
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