Abstract
Chemical etching method shows potential for large-scale and low-cost processed MXenes but incorporates surface terminations such as F&OH that probably deteriorate the lithium storage characteristics. Herein, we propose that tailoring appropriate surface functionalization and the intrinsic electrical properties can dramatically enhance the lithium storage capability of Ti3C2Tx (T stands for F, OH, and O) MXene materials. By carefully controlling the annealing process, the Ti3C2Tx films possess fewer F&OH elements so that with higher conductivity, they are still freestanding and flexible. Density functional theory computations of the low-F&OH-containing Ti3C2Tx show low-ion-diffusion barrier values of 0.34–0.43 eV and a significant increase of Li adsorption energy by 6–30 times compared to those of high-F&OH-containing Ti3C2Tx, suggesting high Li-ion storage and transfer capabilities can be achieved in low-F&OH-containing Ti3C2Tx MXenes. Dramatically, the heteroatom-controlled Ti3C2Tx MXene films show reve...
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