MXenes are known for their exceptional electrical conductivity and surface functionality, gaining interest as promising anode materials for Li-ion batteries. However, conventional 2D multilayered MXenes often exhibit limited electrochemical applicability due to slow ion transport kinetics and low structural stability. Addressing these challenges, this study develops a 3D flower-type double transition metal MXene, Mo2Ti2C3Clx, with precisely engineered in-plane mesoporosity using HF-free Lewis acid-assisted molten salt method, coupled with intercalation and freeze-drying. The molar ratio of Lewis acid to eutectic salts is meticulously controlled to create the mesoporosity, which is preserved through freeze-drying. Molecular dynamics (MD) simulations assess the impact of in-plane pore size on the structure and transport dynamics of electrolyte components. Density functional theory (DFT) shows that chlorine surface functional groups significantly reduce Li-ion diffusion barriers, thereby enhancing ion transport and battery performance. Electrochemical evaluations reveal that small-sized (2-5 nm) mesoporous Mo2Ti2C3Clx achieves a specific capacity of 324 mAh g-1 at 0.2 A g-1 and maintains 97% capacity after 500 cycles at 0.5 A g-1, outperforming larger-pored (10 nm) and non-porous variants. This research highlights a scalable strategy for designing mesoporous materials that optimize ion transport and structural stability, essential for advancing next-generation high-performance energy storage solutions.
Keywords: 3D flower‐type double transition metal MXene; Li‐ion battery; density functional theory; in‐plane mesoporosity; molecular dynamics.
© 2024 The Author(s). Small published by Wiley‐VCH GmbH.