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低浓度DMF/HO混合电解质:水系钾离子电池负极材料的新机遇。

Low Concentration DMF/HO Hybrid Electrolyte: A New Opportunity for Anode Materials in Aqueous Potassium-Ion Batteries.

作者信息

Yuan Xinran, Li Yibo, Zhu Yanan, Deng Wenjun, Li Chang, Zhou Zhuqing, Hu Jun, Zhang Man, Chen Haibiao, Li Rui

机构信息

School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen 518055, China.

出版信息

ACS Appl Mater Interfaces. 2021 Aug 18;13(32):38248-38255. doi: 10.1021/acsami.1c08151. Epub 2021 Aug 3.

Abstract

Superconcentrated "water-in-salt" electrolytes have greatly widened the electrochemical stable window (ESW) of aqueous electrolytes, but they also generate new problems, including high costs, high viscosity, and low conductivity. Here we report a 2 m low concentration electrolyte using an -dimethylformamide/water (DMF/HO) hybrid solvent, which provides a wider ESW (2.89 V) than an aqueous electrolyte (2.66 V) and presents nonflammability, high conductivity, and low viscosity characteristics. In 2 m DMF/HO hybrid electrolyte, the LUMO energy of the DMF solvent (-0.00931 a.u.) is lower than that of HO (-0.00735 a.u.), which could effectively promote the degradation of FSI and lead to stable solid electrolyte interphase formation. As a result, the electrochemical reversibility and cyclability of the KTi(PO)@C (KTP@C) anode in the aqueous electrolyte have been significantly enhanced with the help of DMF addition. Moreover, the KZn(Fe(CN)) (KZnHCF)//KTP@C full potassium-ion battery exhibits highly efficient stability and rate capability with a long cycle performance over 10 000 cycles and delivers a specific discharge capacity of 33 mAh g at a high current density of 20 A g. Low concentrations of DMF/HO hybrid electrolytes can inhibit the hydrogen evolution reaction of aqueous electrolytes, providing more opportunities for the practical application of electrode materials. Not limited to DMF solvent, mixing organic and aqueous solvents will provide more available options and perspectives for improving the energy density and long cycle performance of the aqueous metal-ion battery.

摘要

超浓缩“盐包水”电解质极大地拓宽了水系电解质的电化学稳定窗口(ESW),但也产生了新的问题,包括成本高、粘度高和电导率低。在此,我们报道了一种使用N,N-二甲基甲酰胺/水(DMF/H₂O)混合溶剂的2 m低浓度电解质,其提供了比水系电解质(2.66 V)更宽的ESW(2.89 V),并呈现出不燃性、高电导率和低粘度特性。在2 m DMF/H₂O混合电解质中,DMF溶剂(-0.00931 a.u.)的最低未占分子轨道(LUMO)能量低于H₂O(-0.00735 a.u.),这可以有效地促进双(氟磺酰)亚胺(FSI)的降解并导致形成稳定的固体电解质界面。结果,在添加DMF的帮助下,水系电解质中KTi(PO₄)₃@C(KTP@C)负极的电化学可逆性和循环稳定性得到了显著增强。此外,KZn[Fe(CN)₆](KZnHCF)//KTP@C全钾离子电池表现出高效的稳定性和倍率性能,具有超过10000次循环的长循环性能,并且在20 A g的高电流密度下具有33 mAh g的比放电容量。低浓度的DMF/H₂O混合电解质可以抑制水系电解质的析氢反应,为电极材料的实际应用提供了更多机会。不限于DMF溶剂,混合有机和水系溶剂将为提高水系金属离子电池的能量密度和长循环性能提供更多可用的选择和前景。

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