As a potential cathode material, manganese-based sulfide has recently attracted increasing interest due to its many advantages in aqueous zinc-ion storage. Unfortunately, some challenges such as sluggish kinetics, unstable structure, and controversial phase transition mechanism during the energy storage process hinder its practical application. Herein, inspired by density functional theory (DFT) calculations, a novel 3D sulfur vacancy-rich and heterostructured MnS/MXene aerogel is designed, and used as a cathode for aqueous Zn-ion batteries/hybrid capacitors (ZIBs/ZICs) for the first time. Thanks to the synergistic modification strategy of sulfur vacancies and heterostructures, the as-constructed MnS/MXene//Zn ZIBs exhibit significantly enhanced electrochemical properties, especially outstanding rate capability and cyclic stability. More encouragingly, the as-assembled MnS/MXene//porous carbon (PC) ZICs exhibit an ultrahigh energy density, a high power density, and a splendid cycling lifespan. Most notably, systematic kinetic analyses, ex situ characterizations, and DFT calculations illustrate that MnS/MXene first irreversibly converts into MnO x @ZnMnO 3 /MXene, and then undergoes a reversible conversion from MnO x @ZnMnO 3 /MXene to MnOOH@ZnMn 2 O 4 /MXene, accompanied by the co-insertion/extraction of H + and Zn 2+ . The synergistic modification strategy of sulfur vacancies and heterostructures and the thorough mechanistic study proposed in this work offer valuable guidance for designing and exploiting high-performance cathodes in aqueous zinc-based energy storage devices.
Manganese sulfide (MnS) has been found to be a suitable electrode material for lithium-ion batteries (LIBs) owing to its considerable theoretical capacity, high electrochemical activity, and low discharge voltage platform, while its poor electrical conductivity and severe pulverization caused by volume expansion of the material limit its practical application. To improve the rate performance and cycle stability of MnS in LIBs, the structure-control strategy has been used to design and fabricate new anode materials. Herein, the MnS@MXene@CNF (MMC, CNFs means carbon nanofibers) electrode has been prepared by electrospinning and a subsequent high-temperature annealing process. The MMC electrode exhibits excellent cyclic stability with a capacity retention rate close to 100% after 1000 cycles at 1000 mA/g and an improved rate performance with a specific capacity up to 500 mAh/g at a high current density of 5000 mA/g, much higher than the 308 mAh/g of the MnS@CNF (MC) electrode. The elevated electrochemical performance of the MMC electrode not only benefits from the unique structure of MnS nanoparticles evenly dispersed in the well-designed flexible self-supporting three-dimensional (3D) CNF network but, more importantly, also benefits from the formation of sulfur-bridged Mn–S–C bonds at the MnS/MXene interface. The newly formed bonds between MnS and MXene nanosheets can stabilize the structure of MnS near the interfaces and provide a channel for fast charge transfer, which notably increase both the reversibility and the rate of the conversion reaction during the charge/discharge process. This work may pave a new path for designing stable and self-supporting anodes for high-performance LIBs.
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