Proceedings of nanoGe Fall Meeting19 (NFM19)
Publication date: 18th July 2019
To realize fast-growing field of electric vehicles, rechargeable lithium-sulfur batteries (LSBs) have recently emerged as one of the most exciting alternatives to lithium-ion batteries (LIBs) owing to their higher theoretical energy density, 6 times higher than LIBs and lower cost.[1,2] However, a poor utilization of the active material involved by the electrical insulating character of sulfur and lithium sulfides and a rapid degradation during charge/discharge processes still limit their practical application.[3] Therefore, in this work, an urchin-shaped NiCo2Se4 (u-NCSe) nanostructures as efficient sulfur hosts were synthesized to overcome the limitations of lithium-sulfur batteries (LSBs) using selenization of Ni0.33Co0.67(CO3)0.5OH precursor.[1] The u-NCSe showed a hollow structure with different distribution of Ni, Co and Se, which was proved by electron energy loss spectroscopy (EELS). Meanwhile, the high-resolution transmission electron microscopy (HRTEM) images indicated that the NiCo2Se4 nanostructures had a good crystallinity, in agreement with the cubic phase of NiCo2Se4 (space group: C12/m1). Owing to the hollow structure that can relieve volumetric expansion, a superior electrical conductivity to improve electron transfer, a high polarity to promote absorption of lithium polysulfides (LiPS), and outstanding electrocatalytic activity to accelerate LiPS conversion kinetics, S@u-NCSe delivers outstanding initial capacities up to 1403 mAh/g at 0.1 C and retains 626 mAh/g at 5 C with exceptional rate performance. More significantly, a very low capacity decay rate of only 0.016% per cycle is obtained after 2000 cycles at 3 C. Even at high sulfur loading (3.2 mg/cm2), a reversible capacity of 557 mAh/g is delivered after 600 cycles at 1 C. Density functional theory calculations further confirm the strong interaction between NCSe and LiPS, and cytotoxicity measure-ments prove the biocompatibility of NCSe. This work not only demonstrates that transition metal selenides can be promising candidates as sulfur host materials, but also provides a strategy for the rational design and the development of LSBs with long-life and high-rate electrochemical performance.
This work corresponds to an extension of activities initially performed around the objectives defined by the Helis project which received funding from the European Union’s Horizon 2020 program under the Grant Agreement No. 666221. The authors acknowledge funding from Generalitat de Catalunya2017 SGR 1246 and 2017 SGR 327, the Spanish MINECO projects ENE2016-77798-C4-3-R and ENE2017-85087-C3, and the Zhou Shan Science and Technology Project (2018C21010). C. Zhang and T. Zhang thank the China Scholarship Council (CSC) for scholarship support. IREC acknowledges funding from European Regional Development Funds (ERDF-FEDER Programa Competitivitat de Catalunya 2007–2013). ICN2 was supported by the Severo Ochoa program from Spanish MINECO (Grant No. SEV-2017-0706) and was funded by the CERCA Programme/Generalitat de Catalunya. Part of the present work has been performed in the framework of Universitat Autònoma de Barcelona Materials Science Ph.D. program. This poster is funded by FEDER/Ministerio de Ciencia, Innovación y Universidades – Agencia Estatal de Investigación (ENE2017-85087-C3-3-R).