Abstract

Transition metal chalcogenides (TMCs) have demonstrated great potential in energy storage devices due to their versatile structures and composite functionalities. However, the application of TMCs in potassium-ion batteries (PIBs) suffers from the issues of large volume expansion, polysulfide dissolution, and sluggish kinetics. To overcome these challenges, this work develops nano-flower-like MnS-Co3S4 confined in poly-pyrrole (PPY) carbon nanotube (denoted as MS-CS-PPY) as an excellent anode in PIBs. The nitrogen-doped PPY framework facilitates the interface electron transfer, confines active materials MS-CS effectively, and mitigates the volume change, thus resulting in boosted reaction kinetics and exceptional cycling stability. TMCs induce the surface capacitance and enable the chemical anchoring of the charge/discharge products during the potassium/de-potassium process. Moreover, this work reveals the potassium/de-potassium reaction mechanism, redox kinetics, and solid electrolyte interphase formation of MS-CS-PPY in different electrolytes through theoretical calculations and experimental studies. The solvation ability of electrolytes plays a vital role in manipulating the redox kinetics of the MS-CS-PPY anode material. This study offers feasible strategies for electrode design and electrolyte selection for developing TMCs negative electrodes in future PIBs.

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