Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.039
Publication date: 18th December 2023
Aqueous batteries using non-metallic charge carriers, especially of protons, have recently received significant attention. The proton is the smallest and lightest charge carrier among all cations, which contributes to fast transport kinetics and relatively small structural strain during proton (de)intercalation, leading to promising cycling performance. In recent years, several electrodehost materials with high-rate capability were explored using acidic electrolytes in terms of the proton’s tiny size and unique hopping transport through the hydrogen bond network. For instance, defective Prussian blue analog with high-rate performance (4000 C) and excellent cycling stability were observed. More proton anode materials were explored in metal oxides, mainly including WO3·xH2O, MoO3, H2W2O7, H2Ti3O7, and anatase TiO2. The α-MoO3 has attracted much attention for proton storage owing to its easily modified bilayer structure, fast proton insertion kinetics, and high theoretical-specific capacity. However, the fundamental science of the proton insertion mechanism in α-MoO3 has not been fully understood. Herein, we have uncovered a three-proton intercalation mechanism in α-MoO3 using a specially designed phosphoric acid surfactant lyotropic liquid crystalline electrolyte. The semiconductor-to-metal transition behavior and the expansion of the lattice interlayers of α-MoO3 after trapping one mole of protons were verified experimentally and theoretically. Further investigation of the morphology of α-MoO3 indicated its fracture behavior upon the proton (de)intercalation process, which created ultrafast diffusion channels for hydronium ions. Notably, the first observation of an additional redox behavior at low potential regimes endows a significantly enhanced specific capacity of 362 mAh g-1.
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