Oxygen-Containing Functional Groups Regulating the Carbon/Electrolyte Interfacial Properties Toward Enhanced K^(+)Storage

Oxygen-containing functional groups were found to e ectively boost the K^(+)storage performance of carbonaceous materials,however,the mechanism behind the performance enhancement remains unclear.Herein,we report higher rate capability and better long-term cycle performance employing oxygen-doped graphite oxide(GO)as the anode material for potassium ion batteries(PIBs),compared to the raw graphite.The in situ Raman spectroscopy elucidates the adsorption-intercalation hybrid K^(+)storage mechanism,assigning the capacity enhancement to be mainly correlated with reversible K^(+)adsorption/desorption at the newly introduced oxygen sites.It is unraveled that the C=O and COOH rather than C-O-C and OH groups contribute to the capacity enhancement.Based on in situ Fourier transform infrared(FT-IR)spectra and in situ electrochemical impedance spectroscopy(EIS),it is found that the oxygen-containing functional groups regulate the components of solid electrolyte interphase(SEI),leading to the formation of highly conductive,intact and robust SEI.Through the systematic investigations,we hereby uncover the K^(+)storage mechanism of GO-based PIB,and establish a clear relationship between the types/contents of oxygen functional groups and the regulated composition of SEI.

Stabilizing SEI by cyclic ethers toward enhanced K^(+) storage in graphite

The poor cycling stability of graphite in traditional ester electrolyte limits its applications as anodes for potassium ion batteries(KIBs).Herein,we demonstrate that the introduction of cyclic ether co-solvents into ester electrolytes can remarkably enhance the cycling stability of graphite anodes.The graphite anode in ester electrolyte with cyclic ether could achieve a reversible capacity of 196.1 m Ah g^(-1) after 100 cycles at 0.3 C(1 C=280 m A g^(-1)),about three times higher than those in ester electrolytes with or without linear ether.Compared with the SEI formed in ester electrolytes,the addition of tetrahydrofuran promotes the generation of K_(2)CO_(3) and ethylene oxide oligomers(PEO),of which the K_(2)CO_(3) is expected to be more conductive and PEO is mechanically robust.The more uniform,conductive and stable solid electrolyte interphases(SEIs)on graphite in electrolytes with cyclic ethers contribute to the enhancement of the electrochemical performances of graphite.This work provides a novel design of commercialized electrolytes to achieve high-performance anodes for KIBs,which potentially accelerates the development of KIBs.