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

Oxygen-containing functional groups were found to effectively 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. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-021-00722-3.