Amorphous Heterostructure Derived from Ti₃C₂T_x MXene Towards Superior Lithium-ion Storage

Abstract

Engineering atomic disorder beyond conventional ordered frameworks offers a promising route to unlock the full electrochemical potential of MXenes. Herein, we report the rational design of a heterostructure Ti₃C₂T_x MXene (h-Ti₃C₂T_x) via a controlled ammonium persulfate-induced amorphization strategy. This approach introduces long-range atomic disorder while preserving the MXene layered structure, creating abundant active sites and synergistically enhancing structural robustness. Soft X-ray absorption spectroscopy (sXAS) provided direct evidence of the phase evolution from crystalline MXene (c-Ti₃C₂T_x) to h-Ti₃C₂T_x MXene, revealing the formation of a genuine heterogeneous architecture. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) further confirmed the dual-phase structure, in which crystalline domains coexist with amorphous regions. Complementary selected-area electron diffraction (SAED) established a clear processing-structure relationship, demonstrating a progressive reduction in crystallinity with increasing treatment time. The h-Ti₃C₂T_x electrode delivered a high reversible capacity of 464.4 mA·h·g⁻¹ at 0.1 A/g and outstanding rate capability, retaining 173 mA·h·g⁻¹ at 3.0 A/g, surpassing many previously reported Ti₃C₂T_x MXenes. Ex situ analysis further confirmed the exceptional structural stability of the heterostructured electrode. Overall, this study establishes a spectroscopy-guided heterostructure engineering paradigm for MXenes, providing fundamental insights into crystalline-amorphous coupling and offering a broadly applicable strategy for developing next-generation high-performance Li-ion battery anode materials.

Keywords

MXene / Composite material / Synchrotron radiation characterization / Lithium-ion storage / Structural design / Storage mechanism

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Jilin University, The Editorial Department of Chemical Research in Chinese Universities and Springer-Verlag GmbH