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Edited by: Ping Wu, Nanjing Normal University, China Reviewed by: Yongfeng Yuan, Zhejiang Sci-Tech University, China Wenjia Zhao, Nanjing Agricultural University, China *Correspondence: Yang Xia nanoshine@zjut.edu.cn Specialty section: This article was submitted to Electrochemistry, a section of the journal Frontiers in Chemistry Received: 09 July 2021 Accepted: 19 July 2021 Published: 28 July 2021 Citation: Lu C, Fang R, Wang K, Xiao Z, kumar GG, Gan Y, He X, Huang H, Zhang W and Xia Y (2021) Supercritical CO2 Synthesis of Freestanding Se1-xSx Foamy Cathodes for High- Performance Li-Se1-xSx Battery. Front. Chem. 9:738977. doi: 10.3389/fchem.2021.738977 ORIGINAL RESEARCH published: 28 July 2021 doi: 10.3389/fchem.2021.738977 Supercritical CO2 Synthesis of Freestanding Se1-xSx Foamy Cathodes for High-Performance Li-Se1-xSx Battery Chengwei Lu1, Ruyi Fang1, Kun Wang1, Zhen Xiao2, G. Gnana kumar3, Yongping Gan1, Xinping He1, Hui Huang1, Wenkui Zhang1 and Yang Xia1* 1College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou, China, 2Institute of Optoelectronic Materials and Devices, China Jiliang University, Hangzhou, China, 3Department of Physical Chemistry, School of Chemistry, Madurai Kamaraj University, Madurai, India Selenium-sulfur solid solutions (Se1-xSx) are considered to be a new class of promising cathodic materials for high-performance rechargeable lithium batteries owing to their superior electric conductivity than S and higher theoretical specific capacity than Se. In this work, high- performance Li-Se1-xSx batteries employed freestanding cathodes by encapsulating Se1-xSx in a N-doped carbon framework with three-dimensional (3D) interconnected porous structure (NC@SWCNTs) are proposed. Se1-xSx is uniformly dispersed in 3D porous carbon matrix with the assistance of supercritical CO2 (SC-CO2) technique. Impressively, NC@SWCNTs host not only provides spatial confinement for Se1-xSx and efficient physical/chemical adsorption of intermediates, but also offers a highly conductive framework to facilitate ion/electron transport. More importantly, the Se/S ratio of Se1-xSx plays an important role on the electrochemical performance of Li- Se1-xSx batteries. Benefiting from the rationally designed structure and chemical composition, NC@SWCNTs@Se0.2S0.8 cathode exhibits excellent cyclic stability (632 mA h g−1 at 200 cycle at 0.2 A g−1) and superior rate capability (415mA h g−1 at 2.0A g−1) in carbonate-based electrolyte. This novel NC@SWCNTs@ Se0.2S0.8 cathode not only introduces a new strategy to design high-performance cathodes, but also provides a new approach to fabricate freestanding cathodes towards practical applications of high-energy-density rechargeable batteries. Keywords: Se1-xSx, N-doped carbon foam, supercritical CO2, high areal capacity, Li-Se1-xSx batteries INTRODUCTION Lithium-sulfur (Li-S) batteries are considered as promising next-generation electrochemical energy- storage systems in view of their high theoretical energy density (2600W h kg−1), environmental friendliness and natural richness of sulfur (Yao et al., 2017; Zheng et al., 2020; Yuan et al., 2021a; Yuan et al., 2021b; Sun et al., 2021). Although great progress has been made, the widespread practical application of Li-S battery is still facing issues of the insulation property of natural sulfur (5 × 10−30 S m−1, 25°C), the serious volume effect in the cycle process, and the dissolution of the intermediate polysulfide, leading to the low sulfur utilization, fast capacity decay and poor cycle stability (Zhang et al., 2020). As a congener of element S, Se has similar chemical properties with S, such as high theoretical volumetric capacity (3,253 mA h cm−3, ρ 4.81 g cm−3), which is suitable for mobile devices and Frontiers in Chemistry | www.frontiersin.org 1 July 2021 | Volume 9 | Article 738977PDF Image | Supercritical CO2 Synthesis of Freestanding Se1-xSx Foamy Cathodes for High-Performance Li-Se1-xSx Battery
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