Scalable Synthesis of MAX Phase Precursors toward Titanium-Based MXenes for Lithium-Ion Batteries

ACS Appl Mater Interfaces. 2021 Jun 9;13(22):26074-26083. doi: 10.1021/acsami.1c05889. Epub 2021 Jun 1.

Abstract

MXenes have emerged as one of the most interesting material classes, owing to their outstanding physical and chemical properties enabling the application in vastly different fields such as electrochemical energy storage (EES). MXenes are commonly synthesized by the use of their parent phase, i.e., MAX phases, where "M" corresponds to a transition metal, "A" to a group IV element, and "X" to carbon and/or nitrogen. As MXenes display characteristic pseudocapacitive behaviors in EES technologies, their use as a high-power material can be useful for many battery-like applications. Here, a comprehensive study on the synthesis and characterization of morphologically different titanium-based MXenes, i.e., Ti3C2 and Ti2C, and their use for lithium-ion batteries is presented. First, the successful synthesis of large batches (≈1 kg) of the MAX phases Ti3AlC2 and Ti2AlC is shown, and the underlying materials are characterized mainly by focusing on their structural properties and phase purity. Second, multi- and few-layered MXenes are successfully synthesized and characterized, especially toward their ever-present surface groups, influencing the electrochemical behavior to a large extent. Especially multi- and few-layered Ti3C2 are achieved, exhibiting almost no oxidation and similar content of surface groups. These attributes enable the precise comparison of the electrochemical behavior between morphologically different MXenes. Since the preparation method for few-layered MXenes is adapted to process both active materials in a "classical" electrode paste processing method, a better comparison between both materials is possible by avoiding macroscopic differences. Therefore, in a final step, the aforementioned electrochemical performance is evaluated to decipher the impact of the morphology difference of the titanium-based MXenes. Most importantly, the delamination leads to an increased non-diffusion-limited contribution to the overall pseudocapacity by enhancing the electrolyte access to the redox-active sites.

Keywords: MAX phase; Ti2C; Ti3C2; few- and multi-layered MXene; lithium-ion batteries.