Temperature-induced delamination: A method for uniformly delaminating multilayer Ti3C2Tx via volume changes in low-freezing-point solvents

Titanium-based MXenes, particularly Ti3C2Tx, rank among the most promising two-dimensional (2D) materials owing to their outstanding properties. However, scalable production of large lateral-size Ti3C2Tx monolayers, which could promote their use in polymer-based composites, remains hindered by excessive fragmentation during exfoliation. Here, we report a temperature-induced delamination (TIDE) strategy for sustainable delamination of multilayer Ti3C2Tx, based on reversible volumetric changes in low-freezing-point solvent mixtures during thermal cycling from −20°C to room temperature. After five TIDE cycles with a water/ethanol (1:1 vol) intercalant, the interlayer spacing reaches 6.6 Å, close to the 7.2 Å critical threshold for mild exfoliation predicted by molecular simulations. The resulting single- and few-layer Ti3C2Tx flakes retain lateral sizes above 10 μm with minimal fragmentation, while achieving a conductivity of 6,000 S/cm and a yield of 61 wt %.