title: A Lithium/Polysulfide Battery with Dual-Working Mode Enabled by Liquid Fuel and Acrylate-Based Gel Polymer Electrolyte.
abstract: The low density associated with low sulfur areal loading in the solid-state sulfur cathode of current Li-S batteries is an issue hindering the development of this type of battery. Polysulfide catholyte as a recyclable liquid fuel was proven to enhance both the energy density and power density of the battery. However, a critical barrier with this lithium (Li)/polysulfide battery is that the shuttle effect, which is the crossover of polysulfides and side deposition on the Li anode, becomes much more severe than that in conventional Li-S batteries with a solid-state sulfur cathode. In this work, we successfully applied an acrylate-based gel polymer electrolyte (GPE) to the Li/polysulfide system. The GPE layer can effectively block the detrimental diffusion of polysulfides and protect the Li metal from the side passivation reaction. Cathode-static batteries utilizing 2 M catholyte (areal sulfur loading of 6.4 mg cm-2) present superior cycling stability (727.4 mAh g-1after 500 cycles at 0.2 C) and high rate capability (814 mAh g-1at 2 C) and power density (∼10 mW cm-2), which also possess replaceable and encapsulated merits for mobile devices. In the cathode-flow mode, the Li/polysulfide system with catholyte supplied from an external tank demonstrates further improved power density (∼69 mW cm-2) and stable cycling performance. This novel and simple Li/polysulfide system represents a significant advancement of high energy density sulfur-based batteries for future power sources.
authors.affiliation: Department of Mechanical and Aerospace Engineering, Hong Kong University of Science and Technology , Clear Water Bay, Kowloon, Hong Kong.|Engineering Laboratory for the Next Generation Power and Energy Storage Batteries, Graduate School at Shenzhen, Tsinghua University , Shenzhen 518055, China.|Laboratory of Advanced Materials, School of Materials Science and Engineering, Tsinghua University , Beijing 100084, China.
authors.forename: Ming
authors.initials: M
authors.lastname: Liu
authors.affiliation: Department of Mechanical and Aerospace Engineering, Hong Kong University of Science and Technology , Clear Water Bay, Kowloon, Hong Kong.
authors.forename: Yuxun
authors.initials: Y
authors.lastname: Ren
authors.affiliation: Engineering Laboratory for the Next Generation Power and Energy Storage Batteries, Graduate School at Shenzhen, Tsinghua University , Shenzhen 518055, China.|Laboratory of Advanced Materials, School of Materials Science and Engineering, Tsinghua University , Beijing 100084, China.
authors.forename: Dong
authors.initials: D
authors.lastname: Zhou
authors.affiliation: Department of Mechanical and Aerospace Engineering, Hong Kong University of Science and Technology , Clear Water Bay, Kowloon, Hong Kong.
authors.forename: Haoran
authors.initials: H
authors.lastname: Jiang
authors.affiliation: Engineering Laboratory for the Next Generation Power and Energy Storage Batteries, Graduate School at Shenzhen, Tsinghua University , Shenzhen 518055, China.|Laboratory of Advanced Materials, School of Materials Science and Engineering, Tsinghua University , Beijing 100084, China.
authors.forename: Feiyu
authors.initials: F
authors.lastname: Kang
authors.affiliation: Department of Mechanical and Aerospace Engineering, Hong Kong University of Science and Technology , Clear Water Bay, Kowloon, Hong Kong.
authors.forename: Tianshou
authors.identifier: http://orcid.org/0000-0003-4825-2381
authors.initials: T
authors.lastname: Zhao
keywords: Li/polysulfide battery; energy density; gel polymer electrolyte; liquid fuel; redox flow battery