Linear-Organic-Ions In Situ-Intercalated MoS₂ for Unveiling Capacitive Energy Storage Relies on the Chain Length

Intercalating linear-organic-ions into the MoS₂ interlayer is beneficial for optimizing electrons/ions' capacitive storage behavior. The chain length, as an important parameter of linear organic ions, can lead to differences in the dispersion, polarity, critical micelle concentration of organic ions, and steric hindrance to the growth of MoS₂ nanosheets. Up until now, the relationship between chain length, synthesis of intercalated-MoS₂, and capacitive energy storage has not been unveiled. Herein, we have designed an in situ-intercalation route that is simple, efficient, and high yield for inserting four types of linear organic ions into the interlayer of MoS₂ to synthesize four types of in situ-intercalated MoS₂ samples. After organic-ion intercalation, the expanded interlayer spacing achieved the introduction of intercalation-type pseudocapacitors, as confirmed by ex situ XRD. Improved extra capacitance is verified due to the enlarged ion storage space from a synergistic spatial effect in the broken-shell-hollow ball. Additionally, the generation of high-valent Mo (+5 and +6) and S-vacancies is beneficial for energy storage. More importantly, according to density functional theory (DFT) calculations, as the chain length increases, the number of negative adsorption sites and the total adsorption ability also increase, leading to significantly improved specific capacitance. This work will provide an archetype for the preparation of in situ-intercalated layered materials and unveil capacitive energy storage that relies on the organic-ion chain length.