Solvent Co-intercalation into Few-layered Ti3C2Tx MXenes in Lithium Ion Batteries Induced by Acidic or Basic Post-treatment

MXenes, as an emerging class of 2D materials, display distinctive physical and chemical properties, which are highly suitable for high-power battery applications, such as lithium ion batteries (LIBs). Ti3C2Tx (T-x = O, OH, F, Cl) is one of the most investigated MXenes to this day; however, most scientific research studies only focus on the design of multilayered or monolayer MXenes. Here, we present a comprehensive study on the synthesis of few-layered Ti3C2Tx materials and their use in LIB cells, in particular for high-rate applications. The synthesized Ti3C2Tx MXenes are characterized via complementary XRD, Raman spectroscopy, XPS, EDX, SEM, TGA, and nitrogen adsorption techniques to clarify the structural and chemical changes, especially regarding the surface groups and intercalated cations/water molecules. The structural changes are correlated with respect to the acidic and basic post-treatment of Ti3C2Tx. Furthermore, the detected alterations are put into an electrochemical perspective via galvanostatic and potentiostatic investigations to study the pseudocapacitive behavior of few-layered Ti3C2Tx, exhibiting a stable capacity of 155 mAh g(-1) for 1000 cycles at 5 A g(-1). The acidic treatment of Ti3C2Tx synthesized via the in situ formation of HF through LiF/HCl is able to increase the initial capacity in comparison to the pristine or basic treatment. To gain further insights into the structural changes occurring during (de)lithiation, in situ XRD is applied for LIB cells in a voltage range from 0.01 to 3 V to give fundamental mechanistic insights into the structural changes occurring during the first cycles. Thereby, the increased initial capacity observed for acidic-treated MXenes can be explained by the reduced co-intercalation of solvent molecules.

Automated summary

MXenes, as a type of 2D materials, show unique physical and chemical properties suitable for high-power battery applications, with Ti3C2Tx being one of the most studied variants. Research in this study focuses on synthesizing few-layered Ti3C2Tx materials for use in LIB cells, investigating structural and chemical changes, and exploring the impact of acidic and basic post-treatments on their electrochemical behavior. The findings suggest that the acidic treatment can enhance the initial capacity and stability of the few-layered Ti3C2Tx MXenes in high-rate applications.