title: Rational Integration of Polypropylene/Graphene Oxide/Nafion as Ternary-Layered Separator to Retard the Shuttle of Polysulfides for Lithium-Sulfur Batteries.
abstract: The reversible electrochemical transformation from lithium (Li) and sulfur (S) into Li2 S through multielectron reactions can be utilized in secondary Li-S batteries with very high energy density. However, both the low Coulombic efficiency and severe capacity degradation limits the full utilization of active sulfur, which hinders the practical applications of Li-S battery system. The present study reports a ternary-layered separator with a macroporous polypropylene (PP) matrix layer, graphene oxide (GO) barrier layer, and Nafion retarding layer as the separator for Li-S batteries with high Coulombic efficiency and superior cyclic stability. In the ternary-layered separator, ultrathin layer of GO (0.0032 mg cm(-2) , estimated to be around 40 layers) blocks the macropores of PP matrix, and a dense ion selective Nafion layer with a very low loading amount of 0.05 mg cm(-2) is attached as a retarding layer to suppress the crossover of sulfur-containing species. The ternary-layered separators are effective in improving the initial capacity and the Coulombic efficiency of Li-S cells from 969 to 1057 mAh g(-1) , and from 80% to over 95% with an LiNO3 -free electrolyte, respectively. The capacity degradation is reduced from 0.34% to 0.18% per cycle within 200 cycles when the PP separator is replaced by the ternary-layered separators. This work provides the rational design strategy for multifunctional separators at cell scale to effective utilizing of active sulfur and retarding of polysulfides, which offers the possibility of high energy density Li-S cells with long cycling life.
authors.affiliation: Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.
authors.forename: Ting-Zhou
authors.initials: TZ
authors.lastname: Zhuang
authors.affiliation: Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.
authors.forename: Jia-Qi
authors.initials: JQ
authors.lastname: Huang
authors.affiliation: Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.
authors.forename: Hong-Jie
authors.initials: HJ
authors.lastname: Peng
authors.affiliation: Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.
authors.forename: Lian-Yuan
authors.initials: LY
authors.lastname: He
authors.affiliation: Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.
authors.forename: Xin-Bing
authors.initials: XB
authors.lastname: Cheng
authors.affiliation: Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences, 27 Taoyuan South Road, Taiyuan, 030001, China.
authors.forename: Cheng-Meng
authors.initials: CM
authors.lastname: Chen
authors.affiliation: Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, China.
authors.forename: Qiang
authors.initials: Q
authors.lastname: Zhang
keywords: graphene oxide; lithium-sulfur batteries; polysulfides; separators