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电解质工程对提升镍钴硫钠离子存储性能的作用。

Electrolyte Engineering on Performance Enhancement of NiCo S Anode for Sodium Storage.

机构信息

School of Marine Science and Technology, Harbin Institute of Technology, Weihai, 264209, China.

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education, School of Chemistry and Materials Science, Heilongjiang University, Harbin, 150080, China.

出版信息

Small. 2023 Jun;19(26):e2300188. doi: 10.1002/smll.202300188. Epub 2023 Mar 20.

Abstract

NiCo S is an attractive anode for sodium-ion batteries (SIBs) due to its high capacity and excellent redox reversibility. Practical deployment of NiCo S electrode in SIBs, however, is still hindered by the inferior capacity and unsatisfactory cycling performance, which result from the mismatch between the electrolyte chemistry and electrode. Herein, a functional electrolyte containing 1.0 m NaCF SO in diethylene glycol dimethyl ether (DEGDME) (1.0 m NaCF SO -DEGDME) is developed, which can be readily used for NiCo S anode with high initial coulomb efficiency (96.2%), enhanced cycling performance, and boosted capacities (341.7 mA h g after 250 continuous cycles at the current density of 200 mA g ). The electrochemical tests and related phase characterization combined with density functional theory (DFT) calculation indicate the ether-based electrolyte is more suitable for the NiCo S anode in SIBs due to the formation of a stable electrode-electrolyte interface. Additionally, the importance of the voltage window is also demonstrated to further optimize the electrochemical performance of the NiCo S electrode. The formation of sulfide intermediates during charging and discharging is predicted by combining DFT and verified by in situ XRD and HRTEM. The findings indicate that electrolyte engineering would be an effective way of performance enhancement for sulfides in practical SIBs.

摘要

镍钴硫(NiCoS)因其高容量和优异的氧化还原可逆性而成为钠离子电池(SIBs)的理想阳极。然而,由于电解质化学性质与电极不匹配,NiCoS 电极在 SIBs 中的实际应用仍然受到限制,表现为容量较差和循环性能不理想。在此,开发了一种功能性电解质,其中含有 1.0 m 的双(三氟甲烷磺酰)亚胺钠盐(NaCF3SO2N)在二乙二醇二甲醚(DEGDME)(1.0 m NaCF3SO2N-DEGDME)中,可直接用于 NiCoS 阳极,具有高初始库仑效率(96.2%)、增强的循环性能和提高的容量(在 200 mA g 的电流密度下连续 250 次循环后为 341.7 mA h g)。电化学测试和相关的相表征结合密度泛函理论(DFT)计算表明,基于醚的电解质更适合 SIBs 中的 NiCoS 阳极,因为它形成了稳定的电极-电解质界面。此外,还证明了电压窗口的重要性,以进一步优化 NiCoS 电极的电化学性能。通过结合 DFT 和原位 XRD 和 HRTEM 验证,预测了在充电和放电过程中形成的硫化物中间体。研究结果表明,电解质工程将是提高实际 SIBs 中硫化物性能的有效方法。

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