Lithium-sulfur batteries (LSBs) can replace lithium-ion batteries by delivering a higher specific capacity. However, the areal capacity of current LSBs is low because the intrinsic limitations of sulfur make achieving a high sulfur loading difficult. Herein, the authors report vertically aligned reduced graphene oxide (rGO) with sulfur and poly(ethylene oxide)-based polymer electrolyte double-shell layers (VRG@S@PPE) as a high-loading sulfur cathode. The addition of vapor-grown carbon fiber (VGCF) into rGO is the key to success, as it allows for gas evacuation from internal nano/micropores without structural collapse, enabling perfect double-shell layer contact. Owing to the anisotropic rGO lamellar structure that enables straightforward ion/electron transport and provides numerous active sites, sulfur-infiltrated rGO reinforced via VGCF (VRG@S) exhibits a high capacity of 998 mAh g−1 after 100 cycles at 0.1 C under high sulfur loading (6 mg cm−2). Interestingly, an additional polymer electrolyte layer further increases the cycle retention (1005 and 718 mAh g−1 after 100 cycles at 0.1 and 1 C, respectively), because intimate contact between the solid polymer electrolyte and sulfur could suppress the loss of sulfur due to lithium polysulfide (LPS) shuttling or volume change during lithiation/delithiation. Therefore, it is possible to realize safe and stable quasi-solid-state LSBs with high sulfur loading.
Bibliographical noteFunding Information:
This work was supported by a National Research Foundation of Korea (NRF) Grant funded by the Ministry of Science, ICT, and Future Planning, South Korea (2018M3D1A1058744, 2022R1A2C3003319, 2022R1C1C1006019). This research was supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (2020R1A6A1A03045059). This work was supported by the National Research Foundation of Korea Grant funded by the Korean Government(MOE). The authors thank the Korea Basic Science Institute for the technical support.
© 2022 The Authors. Advanced Science published by Wiley-VCH GmbH.
- 3D reduced graphene oxide arrays
- free-standing electrodes
- gel-polymer electrolytes
- high areal mass loading
- quasi-solid-state lithium-sulfur batteries
ASJC Scopus subject areas
- Medicine (miscellaneous)
- Chemical Engineering(all)
- Materials Science(all)
- Biochemistry, Genetics and Molecular Biology (miscellaneous)
- Physics and Astronomy(all)